\r\n\tWe accept scientific papers which can be presented as original research papers and review papers. The required length of the full chapters is 10-20 pages and the chapters should be original works (not republished). \r\n\tAs a self-contained collection of scholarly papers, the book will target an audience of practicing researchers, academics, Ph.D. students and other scientists. Since it will be published as an Open Access publication, it will allow unrestricted online access to chapters with no reading or subscription fees.
",isbn:null,printIsbn:"979-953-307-X-X",pdfIsbn:null,doi:null,price:0,priceEur:0,priceUsd:0,slug:null,numberOfPages:0,isOpenForSubmission:!1,hash:"a8274c7a57830fae9cfa2dd00780184f",bookSignature:"Associate Prof. Arpit Sand",publishedDate:null,coverURL:"https://cdn.intechopen.com/books/images_new/8505.jpg",keywords:"Applications, PEG, Biotechnical, Biomedical, Water Structure, Cell Fusion, DSC Measurement, Phase Diagram, NMR Spectroscopy, Protein Interaction, Grafted PEG Surface, Monte Carlo ,Protein Hybrid Catalyst, Nano Protein ,Metal Complex",numberOfDownloads:null,numberOfWosCitations:0,numberOfCrossrefCitations:0,numberOfDimensionsCitations:0,numberOfTotalCitations:0,isAvailableForWebshopOrdering:!0,dateEndFirstStepPublish:"May 8th 2019",dateEndSecondStepPublish:"September 2nd 2019",dateEndThirdStepPublish:"November 1st 2019",dateEndFourthStepPublish:"January 20th 2020",dateEndFifthStepPublish:"March 20th 2020",remainingDaysToSecondStep:"a year",secondStepPassed:!0,currentStepOfPublishingProcess:5,editedByType:null,kuFlag:!1,biosketch:null,coeditorOneBiosketch:null,coeditorTwoBiosketch:null,coeditorThreeBiosketch:null,coeditorFourBiosketch:null,coeditorFiveBiosketch:null,editors:[{id:"287032",title:"Associate Prof.",name:"Arpit",middleName:null,surname:"Sand",slug:"arpit-sand",fullName:"Arpit Sand",profilePictureURL:"https://mts.intechopen.com/storage/users/287032/images/system/287032.jpg",biography:"Dr. Arpit Sand is currently Associate Professor in the Department of Chemistry, Manav Rachna University Faridabad India. He received his B.Sc. in Science and M.Sc. in Chemistry from the University of Allahabad, Allahabad, India. Dr. Arpit received his Ph.D. degree in Chemistry from the University of Allahabad, Allahabad, India, in 2010. Dr. Sand is an editorial board member for numerous recognized publishers. In addition, he is a reviewer for multiple international journals. He has authored more than 24 international research articles.",institutionString:"Manav Rachna International University",position:null,outsideEditionCount:0,totalCites:0,totalAuthoredChapters:"0",totalChapterViews:"0",totalEditedBooks:"0",institution:null}],coeditorOne:null,coeditorTwo:null,coeditorThree:null,coeditorFour:null,coeditorFive:null,topics:[{id:"8",title:"Chemistry",slug:"chemistry"}],chapters:null,productType:{id:"1",title:"Edited Volume",chapterContentType:"chapter",authoredCaption:"Edited by"},personalPublishingAssistant:{id:"304289",firstName:"Rebekah",lastName:"Pribetic",middleName:null,title:"Ms.",imageUrl:"https://mts.intechopen.com/storage/users/304289/images/13255_n.png",email:"rebekah@intechopen.com",biography:null}},relatedBooks:[{type:"book",id:"1591",title:"Infrared Spectroscopy",subtitle:"Materials Science, Engineering and Technology",isOpenForSubmission:!1,hash:"99b4b7b71a8caeb693ed762b40b017f4",slug:"infrared-spectroscopy-materials-science-engineering-and-technology",bookSignature:"Theophile Theophanides",coverURL:"https://cdn.intechopen.com/books/images_new/1591.jpg",editedByType:"Edited by",editors:[{id:"37194",title:"Dr.",name:"Theophanides",surname:"Theophile",slug:"theophanides-theophile",fullName:"Theophanides Theophile"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"3092",title:"Anopheles mosquitoes",subtitle:"New insights into malaria vectors",isOpenForSubmission:!1,hash:"c9e622485316d5e296288bf24d2b0d64",slug:"anopheles-mosquitoes-new-insights-into-malaria-vectors",bookSignature:"Sylvie Manguin",coverURL:"https://cdn.intechopen.com/books/images_new/3092.jpg",editedByType:"Edited by",editors:[{id:"50017",title:"Prof.",name:"Sylvie",surname:"Manguin",slug:"sylvie-manguin",fullName:"Sylvie Manguin"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"3161",title:"Frontiers in Guided Wave Optics and Optoelectronics",subtitle:null,isOpenForSubmission:!1,hash:"deb44e9c99f82bbce1083abea743146c",slug:"frontiers-in-guided-wave-optics-and-optoelectronics",bookSignature:"Bishnu Pal",coverURL:"https://cdn.intechopen.com/books/images_new/3161.jpg",editedByType:"Edited by",editors:[{id:"4782",title:"Prof.",name:"Bishnu",surname:"Pal",slug:"bishnu-pal",fullName:"Bishnu Pal"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"72",title:"Ionic Liquids",subtitle:"Theory, Properties, New Approaches",isOpenForSubmission:!1,hash:"d94ffa3cfa10505e3b1d676d46fcd3f5",slug:"ionic-liquids-theory-properties-new-approaches",bookSignature:"Alexander Kokorin",coverURL:"https://cdn.intechopen.com/books/images_new/72.jpg",editedByType:"Edited by",editors:[{id:"19816",title:"Prof.",name:"Alexander",surname:"Kokorin",slug:"alexander-kokorin",fullName:"Alexander Kokorin"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"1373",title:"Ionic Liquids",subtitle:"Applications and Perspectives",isOpenForSubmission:!1,hash:"5e9ae5ae9167cde4b344e499a792c41c",slug:"ionic-liquids-applications-and-perspectives",bookSignature:"Alexander Kokorin",coverURL:"https://cdn.intechopen.com/books/images_new/1373.jpg",editedByType:"Edited by",editors:[{id:"19816",title:"Prof.",name:"Alexander",surname:"Kokorin",slug:"alexander-kokorin",fullName:"Alexander Kokorin"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"57",title:"Physics and Applications of Graphene",subtitle:"Experiments",isOpenForSubmission:!1,hash:"0e6622a71cf4f02f45bfdd5691e1189a",slug:"physics-and-applications-of-graphene-experiments",bookSignature:"Sergey Mikhailov",coverURL:"https://cdn.intechopen.com/books/images_new/57.jpg",editedByType:"Edited by",editors:[{id:"16042",title:"Dr.",name:"Sergey",surname:"Mikhailov",slug:"sergey-mikhailov",fullName:"Sergey Mikhailov"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"371",title:"Abiotic Stress in Plants",subtitle:"Mechanisms and Adaptations",isOpenForSubmission:!1,hash:"588466f487e307619849d72389178a74",slug:"abiotic-stress-in-plants-mechanisms-and-adaptations",bookSignature:"Arun Shanker and B. Venkateswarlu",coverURL:"https://cdn.intechopen.com/books/images_new/371.jpg",editedByType:"Edited by",editors:[{id:"58592",title:"Dr.",name:"Arun",surname:"Shanker",slug:"arun-shanker",fullName:"Arun Shanker"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"878",title:"Phytochemicals",subtitle:"A Global Perspective of Their Role in Nutrition and Health",isOpenForSubmission:!1,hash:"ec77671f63975ef2d16192897deb6835",slug:"phytochemicals-a-global-perspective-of-their-role-in-nutrition-and-health",bookSignature:"Venketeshwer Rao",coverURL:"https://cdn.intechopen.com/books/images_new/878.jpg",editedByType:"Edited by",editors:[{id:"82663",title:"Dr.",name:"Venketeshwer",surname:"Rao",slug:"venketeshwer-rao",fullName:"Venketeshwer Rao"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"4816",title:"Face Recognition",subtitle:null,isOpenForSubmission:!1,hash:"146063b5359146b7718ea86bad47c8eb",slug:"face_recognition",bookSignature:"Kresimir Delac and Mislav Grgic",coverURL:"https://cdn.intechopen.com/books/images_new/4816.jpg",editedByType:"Edited by",editors:[{id:"528",title:"Dr.",name:"Kresimir",surname:"Delac",slug:"kresimir-delac",fullName:"Kresimir Delac"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"3621",title:"Silver Nanoparticles",subtitle:null,isOpenForSubmission:!1,hash:null,slug:"silver-nanoparticles",bookSignature:"David Pozo Perez",coverURL:"https://cdn.intechopen.com/books/images_new/3621.jpg",editedByType:"Edited by",editors:[{id:"6667",title:"Dr.",name:"David",surname:"Pozo",slug:"david-pozo",fullName:"David Pozo"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}}]},chapter:{item:{type:"chapter",id:"17640",title:"Modern Synthesis and Thermoresponsivity of Polyphosphoesters",doi:"10.5772/18538",slug:"modern-synthesis-and-thermoresponsivity-of-polyphosphoesters",body:'\n\t\t
\n\t\t\t
1. Introduction
\n\t\t\t
There has been a great deal of interest in polyphosphoesters, which are biodegradable through hydrolysis and possibly through enzymatic digestion of phosphate linkages under physiological conditions (Renier et al., 1997). Biodegradable polyphosphoesters appear interesting for biological and pharmaceutical applications because of their biocompatibility and structural similarities to naturally occurring nucleic and teichoic acids. Recently, there have been interesting studies of polyphosphoesters used in biomedical applications (Wang et al., 2009). In particular, the advantages of polyphosphoesters for use in the field of tissue engineering as scaffolds and gene carriers was elucidated (Wan et al., 2001; Wang et al., 2002; Huang et al., 2004; Ren et al., 2010).
\n\t\t\t
Figure 1.
Schematic contents of this chapter.
\n\t\t\t
\n\t\t\t\tFigure 1 is a schematic representation of the contents of this chapter describing current research on polyphosphoesters. Although polyphosphoesters have a relatively long history, well-defined synthesis of the polymers has not been well explained. For use in medical applications such as drug delivery systems, understanding the synthetic process of polymers with narrow molecular weight distribution may be quite important to obtain reproducibility. The first part of this chapter discusses the controlled synthesis of polyphosphoesters.
\n\t\t\t
In comparison with conventional biodegradable polymers, the molecular functionalization of polyphosphoesters is easier because varied cyclic phosphoesters, which work as monomers, can be obtained by a simple condensation reaction between alcohol and chloro cyclic phosphoesters. That is, theoretically, any alcohol can be introduced into polyphosphoesters. Here, a biodegradable macroinitiator and macrocrosslinker based on polyphosphoesters are described. They can be used as building blocks for preparing polymer blends and hydrogels.
\n\t\t\t
We have also recently found that polyphosphoesters show thermoresponsivity in aqueous media. This polymer solution makes a lower critical solution temperature (LCST) type coacervate. The phenomenon is strongly influenced by the structure and molecular weight of the polymers and the solvent condition. The basic thermoresponsive properties of polyphosphoesters are summarized in this chapter. Enzyme-responsive polyphosphoesters are also introduced.
\n\t\t
\n\t\t
\n\t\t\t
2. Synthesis of well-defied polyphosphoesters and incorporation of functional groups into polymers
\n\t\t\t
A variety of synthetic routes for polyphosphoesters have been reported including ring-opening polymerization (ROP) (Libiszowski et al., 1978; Pretula et al., 1986), polycondensation (Richard et al, 1991), transesterfication (Pretula et al., 1999; Myrex et al., 2003), and enzymatic polymerization (Wen et al., 1998). Since the pioneering experiments by the Penczek group (Penczek & Klosinski, 1990), the ROP of cyclic phosphate has been studied for more than three decades and various polymers having a phosphoester backbone have been designed. The ROP of cyclic phosphoesters is the most common process used to obtain polyphosphoesters. This is because a variety of polyphosphoesters can be designed in comparison with conventional biodegradable polymers because cyclic phosphoesters are obtained as monomers from the condensation of alcohol and 2-chloro-2-oxo-1,3,2-dioxaphospholane (Katuiyhski et al., 1976).
\n\t\t\t
\n\t\t\t\t
2.1. Synthesis of polyphosphoesters using organocatalysts
\n\t\t\t\t
For the ROP of cyclic phosphoesters, metallic compounds are commonly used as initiators or polymerization catalysts (Penczek et al., 1990; Libiszowski et al., 1978; Pretula et al., 1986; Xiao et al., 2006). Although the polymerization processes are very successful in producing polyphosphoesters, the metal compounds are environmentally sensitive and a lack of residual metal contaminants is required in biomedical applications. Recently, organocatalysts have been the focus of the modern synthetic processes of polyesters, polycarbonates, and silicones (Kamber et al., 2007). One of the most successful procedures for making biodegradable polymers is polymerization using guanidine and amidine bases, both in bulk and in solution. Nederberg and Hedrick prepared poly(trimethylene carbonate (TMC)) (PTMC) with the base catalysts in the presence of benzyl alcohol (Nederberg et al., 2007). Excellent controlled polymerization conditions were present with several catalysts, and PTMCs with relatively high molecular weight, narrow distribution, and high yield were obtained. We have recently recognized that organocatalysts have high potency for the ROP of cyclic phosphoesters (Iwasaki et al., 2010).
\n\t\t\t\t
Scheme 1.
Synthetic route of PIPP. (Reproduced from Iwasaki et al., (2010)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138, Copyright (2010), with permission from the American Chemical Society)
\n\t\t\t\t
Poly(2-isopropoxy-2-oxo-1,3,2-dioxaphospholane) (PIPPn; n is degree of polymerization) was synthesized by ROP using an organocatalyst as an initiator in the presence of 2-hydroxyethyl-2’-bromoisobutyrate (HEBB) (Scheme 1). In the case of 1,8-diazabicyclo[5,4,0]undec-7-ene (DBU), polymerization was homogeneously performed in a solvent-free condition. In contrast, a small amount of toluene was used for dissolving 1,5,7-triazabicyclo[4,4,0]dec-5-ene (TBD) to make a homogeneous solution. The results of PIPP synthesis are summarized in Table 1. Twenty mmoles of IPP was first introduced into a polymerization tube under an argon gas atmosphere at 0°C, and then a given amount of HEBB was added to the tube. Finally, a given amount of organocatalyst was introduced. Polymerization was carried out at 0°C. The range of molecular weights was approximately 2.0 x 103 to 3.0 x 104 g/mol by gel-permeation chromatography (GPC) using a calibration curve based on linear polystyrene standards with chloroform as the mobile phase. In every case, the molecular weight distribution was lower than 1.10. Under each condition, the molecular weights of the synthetic polymers agreed with the theoretical values.
\n\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
Code
\n\t\t\t\t\t\t\t
Catalyst
\n\t\t\t\t\t\t\t
[M]0/[I]
\n\t\t\t\t\t\t\t
HEBB (mmol)
\n\t\t\t\t\t\t\t
Catalyst (mmol)
\n\t\t\t\t\t\t\t
Time (min)
\n\t\t\t\t\t\t\t
Conv. (%)
\n\t\t\t\t\t\t\t
\n\t\t\t\t\t\t\t\tM\n\t\t\t\t\t\t\t\tn\n\t\t\t\t\t\t\t\t x 10-3\n\t\t\t\t\t\t\t
\n\t\t\t\t\t\t\t\tM\n\t\t\t\t\t\t\t\tn(Theo)\n\t\t\t\t\t\t\t\t x 10-3\n\t\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP13
\n\t\t\t\t\t\t\t
DBU
\n\t\t\t\t\t\t\t
25
\n\t\t\t\t\t\t\t
0.80
\n\t\t\t\t\t\t\t
1.20
\n\t\t\t\t\t\t\t
60
\n\t\t\t\t\t\t\t
52.8
\n\t\t\t\t\t\t\t
2.4
\n\t\t\t\t\t\t\t
1.03
\n\t\t\t\t\t\t\t
2.2
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP32
\n\t\t\t\t\t\t\t
DBU
\n\t\t\t\t\t\t\t
50
\n\t\t\t\t\t\t\t
0.40
\n\t\t\t\t\t\t\t
0.60
\n\t\t\t\t\t\t\t
90
\n\t\t\t\t\t\t\t
52.7
\n\t\t\t\t\t\t\t
4.7
\n\t\t\t\t\t\t\t
1.07
\n\t\t\t\t\t\t\t
4.4
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP50
\n\t\t\t\t\t\t\t
DBU
\n\t\t\t\t\t\t\t
100
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
0.30
\n\t\t\t\t\t\t\t
300
\n\t\t\t\t\t\t\t
50.8
\n\t\t\t\t\t\t\t
7.7
\n\t\t\t\t\t\t\t
1.09
\n\t\t\t\t\t\t\t
8.4
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP48
\n\t\t\t\t\t\t\t
TBD
\n\t\t\t\t\t\t\t
50
\n\t\t\t\t\t\t\t
0.40
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
20
\n\t\t\t\t\t\t\t
81.2
\n\t\t\t\t\t\t\t
8.2
\n\t\t\t\t\t\t\t
1.06
\n\t\t\t\t\t\t\t
6.7
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP77
\n\t\t\t\t\t\t\t
TBD
\n\t\t\t\t\t\t\t
100
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
20
\n\t\t\t\t\t\t\t
80.7
\n\t\t\t\t\t\t\t
13.0
\n\t\t\t\t\t\t\t
1.09
\n\t\t\t\t\t\t\t
13.4
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP117
\n\t\t\t\t\t\t\t
TBD
\n\t\t\t\t\t\t\t
150
\n\t\t\t\t\t\t\t
0.13
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
20
\n\t\t\t\t\t\t\t
75.5
\n\t\t\t\t\t\t\t
16.9
\n\t\t\t\t\t\t\t
1.07
\n\t\t\t\t\t\t\t
18.8
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
PIPP174
\n\t\t\t\t\t\t\t
TBD
\n\t\t\t\t\t\t\t
200
\n\t\t\t\t\t\t\t
0.10
\n\t\t\t\t\t\t\t
0.20
\n\t\t\t\t\t\t\t
20
\n\t\t\t\t\t\t\t
90.3
\n\t\t\t\t\t\t\t
28.9
\n\t\t\t\t\t\t\t
1.05
\n\t\t\t\t\t\t\t
30.0
\n\t\t\t\t\t\t
\n\t\t\t\t\t
Table 1.
Synthetic results of PIPPn. (Reproduced from Iwasaki et al., (2010)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138, Copyright (2010), with permission from the American Chemical Society)
\n\t\t\t\t
\n\t\t\t\t\tFigure 2 shows the number-averaged molecular weight (M\n\t\t\t\t\tn) versus monomer conversion for the polymerization of IPP by using DBU as a catalyst. The plot of M\n\t\t\t\t\tn vs. conversion was linear up to 60% conversion. The linearity of the plot suggests that the number of macromolecules in the reaction system was constant during polymerization. The molecular weight distribution of PIPP was narrow and stable during polymerization. The mechanism of ROP with organocatalysts was characterized using 1H NMR by Hedrick and co-workers (Nederberg et al., 2007; Pratt et al., 2006). They indicated that DBU and TBD form hydrogen bonds to the alcohol of an initiator. ROP of IPP with DBU then occurs through a quasi-anionic polymerization mechanism by activation of the alcohol of the initiator. In contrast, the increase in monomer conversion for the polymerization of IPP between DBU and TBD was significantly different. When TBD was used as a catalyst, the conversion of PIPP reached a level of more than 75% within 20 min. The heightened activity of TBD for the polymerization of lactone and TMC was also observed (Nederberg et al., 2007).
\n\t\t\t\t
Figure 2.
Plot of M\n\t\t\t\t\t\t\tw/M\n\t\t\t\t\t\t\tn and M\n\t\t\t\t\t\t\tn versus monomer conversion for the polymerization of 2-isopropoxy-2-oxo-1,3,2-dioxaphospholane by using 1,8-diazabicyclo[5,4,0]undec-7-ene as a catalyst. Lines suggest the theoretical amount of each polymerization condition. (Reproduced from Iwasaki et al., (2010)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138, Copyright (2010), with permission from the American Chemical Society)
\n\t\t\t
\n\t\t\t
\n\t\t\t\t
2.2. Polyphosphoester macroinitiators
\n\t\t\t\t
Atom transfer radical polymerization (ATRP) has great ability to control the molecular architecture of synthetic polymers and is an exceptionally robust method of producing block or graft copolymers (Matyjaszewski & Xia, 2001). However, the still limited design of biodegradable amphiphilic polymers has been performed via ATRP. Polyphosphoesters bearing 2-bromo-isobutyryl groups as novel biodegradable macroinitiators for ATRP were then synthesized and amphiphilic polymers with well–defined hydrophilic graft chains were prepared (Iwasaki & Akiyoshi, 2004).
\n\t\t\t\t
A cyclic phosphoester bearing bromoisobutyrate, 2-(2-oxo,1,3,2-dioxaphospholoyloxy) ethyl-2’-bromoisobutyrate (OPBB), was obtained from the reaction of HEBB and 2-chloro-2-oxo-1,3,2-dioxaphosphorane (COP). Poly(IPP-co-OPBB) (PIxBry (Scheme 2); x:IPP (mol%), y: OPBB (mol%)) was synthesized by ring-opening polymerization using triisobutyl aluminum (TIBA) as an initiator. The chemical structure and synthetic results of the polyphosphoesters are shown in Scheme 2 and Table 2, respectively. Polymerization was homogeneously performed by a solvent-free reaction. As indicated in Table 2, the composition of each monomer unit could be controlled by the feed. The M\n\t\t\t\t\tw of the polyphosphoester was 3.1 x 104 to 3.9 x 104 g/mol. The absolute molecular weights of PIBr2 and PIBr5 determined by MALLS were 3.4 x 104 and 3.7 x 104, respectively.
\n\t\t\t\t
ATRP of 2-methacryloyloxyethyl phosphorylcholine (MPC) from macroinitiator polyphosphoesters was carried out in an ethanol solution. Figure 3 shows the number of MPC units in a graft chain of PIBr2-g-PMPC and PIBr5-g-PMPC as determined by 1H NMR. The numbers were linearly increased with an increase in the duration of polymerization. The slope of the PIBr2-g-PMPC was much greater than that of PIBr5-g-PMPC. The rates of polymerization decreased with graft density.
\n\t\t\t\t
Scheme 2.
Synthetic route of polyphosphoester bearing bromoisobutyrate (PIBr). (Reproduced from Iwasaki et al., (2004)\n\t\t\t\t\t\t\tMacromolecules, Vol. 37, No. 20, pp. 7637-7642, Copyright (2004), with permission from the American Chemical Society)
Synthetic results of PIBr. (Reproduced from Iwasaki et al., (2004)\n\t\t\t\t\t\t\tMacromolecules, Vol. 37, No. 20, pp. 7637-7642, Copyright (2004), with permission from the American Chemical Society)
\n\t\t\t\t
Figure 3.
Change in number of units of MPC in a graft chain during ATRP. (Circle): PIBr3-g-PMPC; (Square): PIBr5-g-PMPC. (Reproduced from Iwasaki et al., (2004)\n\t\t\t\t\t\t\tMacromolecules, Vol. 37, No. 20, pp. 7637-7642, Copyright (2004), with permission from the American Chemical Society)
\n\t\t\t\t
The transition point of the surface tension increased with an increase in the molecular weight and density of PMPC. Typical examples for the concentrations of PIBr3-g-PMPC71[1] - and PIBr5-g-PMPC115 were 8.6 x 10-3 g/dL and 2.3 x 10-3 g/dL, respectively. A decrease in surface tensions was observed on every graft copolymer. The surface tensions were influenced by the density and molecular weight of PMPC.
\n\t\t\t\t
Based on MALLS analysis for associative PIBr3-g-PMPC71, the molecular weight of the polymeric associate was 91.1 x 104. From the data in Figure 3, the molecular weight of PIBr3-g-PMPC71 can be estimated at 13.6 x 104. Thus, the association number of the PIBr3-g-PMPC71 was 6.7. For PIBr5-g-PMPC, the association number was 1.5, that is, it is almost a “unimer-micelle.” Figure 4 shows schematic representations of the polymeric associates of PIBr2-g-PMPC12 and PIBr5-g-PMPC115.
\n\t\t\t\t
In an acidic medium, the loss of molecular weight of the graft copolymer was observed as being less; degradation remarkably occurred after 50 days of soaking. Under physiological pH conditions, the molecular weight of the PIBr-g-PMPC decreased from 15.6 x 104 (GPC data) to 12.7 x 104 after 50 days. Under a basic condition, the polyphosphoester degraded almost completely within 3 days. After soaking in pH11.0, the PIBr2-g-PMPC71 and PIBr5-g-PMPC115 polymers had molecular weights of 2.4 x 10-4 and 3.1 x 10-4 (M\n\t\t\t\t\tw/M\n\t\t\t\t\tn=1.2), respectively, as determined by GPC. These polymers were identified as PMPC by 1H NMR (data not shown). Although a basic condition (pH11.0) is not a physiological condition, we chose the optimal pH to characterize the degradation behavior of polyphosphoesters in a relatively short period. Under an acidic condition (pH 4.0), the hydrolysis of PIBr was slow. In contrast, under a basic condition (pH 11.0), the PIBr was completely degraded in only 3 days.
\n\t\t\t\t
Figure 4.
Schematic representation of PIBr and PIBr-g-PMPC. (Reproduced from Iwasaki et al., (2004)\n\t\t\t\t\t\t\tMacromolecules, Vol. 37, No. 20, pp. 7637-7642, Copyright (2004), with permission from the American Chemical Society)
\n\t\t\t\t
The PIPPn shown in Scheme 1 also works as a macroinitiator because it has bromoisobutyrate at the end. Using PIPPn, well-defined block copolymers can be obtained by ATRP (Iwasaki et al., 2010).
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\n\t\t\t
\n\t\t\t\t
2.3. Polyphosphoester macrocrosslinkers
\n\t\t\t\t
Biomaterials have an enormous impact on human health care. They are widely used in biomedical applications, including drug delivery devices and tissue engineering matrices (Lin et al., 2003). Specifically, hydrogels are included in the more recent development of biomaterials because they can absorb significant amounts of water and are as flexible as soft tissue, which minimizes their potential for irritating surrounding tissue. In order to obtain synthetic cellular matrices offering both biocompatibility and biodegradability, a novel porous biodegradable MPC polymer hydrogel crosslinked with polyphosphoesters was prepared with a gas-forming technique (Iwasaki et al., 2003; Iwasaki et al., 2004; Wachiralarpphaithoon et al., 2007).
\n\t\t\t\t
Scheme 3.
Synthetic route of PIOP. (Reproduced from Wachiralarpphaithoon et al., (2007)\n\t\t\t\t\t\t\tBiomaterials, Vol. 28, No. 6, pp. 984-993, Copyright (2007), with permission from Elsevier)
\n\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
Code
\n\t\t\t\t\t\t\t
PIOP:MPC (%)
\n\t\t\t\t\t\t\t
Potassium hydrogen carbonate size range (µm)
\n\t\t\t\t\t\t\t
Swelling ratio (%)
\n\t\t\t\t\t\t\t
Elastic modulus (x 104 Pa)
\n\t\t\t\t\t\t\t
Porosity (%)
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G1
\n\t\t\t\t\t\t\t
0.5:99.5
\n\t\t\t\t\t\t\t
-
\n\t\t\t\t\t\t\t
1519±208
\n\t\t\t\t\t\t\t
2.47±0.47
\n\t\t\t\t\t\t\t
95.0±0.3
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G1A
\n\t\t\t\t\t\t\t
0.5:99.5
\n\t\t\t\t\t\t\t
500-300
\n\t\t\t\t\t\t\t
1576±191
\n\t\t\t\t\t\t\t
0.06±0.01
\n\t\t\t\t\t\t\t
98.4±0.4
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G1B
\n\t\t\t\t\t\t\t
0.5:99.5
\n\t\t\t\t\t\t\t
300-250
\n\t\t\t\t\t\t\t
1549±502
\n\t\t\t\t\t\t\t
0.05±0.01
\n\t\t\t\t\t\t\t
98.2±0.1
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G1C
\n\t\t\t\t\t\t\t
0.5:99.5
\n\t\t\t\t\t\t\t
250-150
\n\t\t\t\t\t\t\t
1547±665
\n\t\t\t\t\t\t\t
0.04±0.00
\n\t\t\t\t\t\t\t
97.8±0.2
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G2
\n\t\t\t\t\t\t\t
1:99
\n\t\t\t\t\t\t\t
-
\n\t\t\t\t\t\t\t
804±128
\n\t\t\t\t\t\t\t
3.08±0.77
\n\t\t\t\t\t\t\t
92.7±0.6
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G2A
\n\t\t\t\t\t\t\t
1:99
\n\t\t\t\t\t\t\t
500-300
\n\t\t\t\t\t\t\t
963±129
\n\t\t\t\t\t\t\t
0.18±0.01
\n\t\t\t\t\t\t\t
96.4±0.3
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G2B
\n\t\t\t\t\t\t\t
1:99
\n\t\t\t\t\t\t\t
300-250
\n\t\t\t\t\t\t\t
957±153
\n\t\t\t\t\t\t\t
0.21±0.02
\n\t\t\t\t\t\t\t
96.5±0.1
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G2C
\n\t\t\t\t\t\t\t
1:99
\n\t\t\t\t\t\t\t
250-150
\n\t\t\t\t\t\t\t
977±26
\n\t\t\t\t\t\t\t
0.26±0.01
\n\t\t\t\t\t\t\t
96.7±0.2
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G3
\n\t\t\t\t\t\t\t
2.5:97.5
\n\t\t\t\t\t\t\t
-
\n\t\t\t\t\t\t\t
357±103
\n\t\t\t\t\t\t\t
10.10±3.26
\n\t\t\t\t\t\t\t
86.0±1.3
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G3A
\n\t\t\t\t\t\t\t
2.5:97.5
\n\t\t\t\t\t\t\t
500-300
\n\t\t\t\t\t\t\t
518±40
\n\t\t\t\t\t\t\t
2.61±0.23
\n\t\t\t\t\t\t\t
96.2±0.1
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G3B
\n\t\t\t\t\t\t\t
2.5:97.5
\n\t\t\t\t\t\t\t
300-250
\n\t\t\t\t\t\t\t
523±183
\n\t\t\t\t\t\t\t
2.61±0.25
\n\t\t\t\t\t\t\t
95.8±0.1
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
G3C
\n\t\t\t\t\t\t\t
2.5:97.5
\n\t\t\t\t\t\t\t
250-150
\n\t\t\t\t\t\t\t
512±133
\n\t\t\t\t\t\t\t
2.65±0.01
\n\t\t\t\t\t\t\t
94.8±0.2
\n\t\t\t\t\t\t
\n\t\t\t\t\t
Table 3.
Synthetic condition and properties of hydrogels. (Reproduced from Wachiralarpphaithoon et al., (2007)\n\t\t\t\t\t\t\tBiomaterials, Vol. 28, No. 6, pp. 984-993, Copyright (2007), with permission from Elsevier)
\n\t\t\t\t
The synthetic route of the macrocrosslinker, PIOP, was also synthesized using TIBA as an initiator (Scheme 4). The molecular weight of PIOP was 1.1 x 104 (M\n\t\t\t\t\tw/M\n\t\t\t\t\tn=1.1). The calculated number of 2-(2-oxo-1,3,2-dioxaphosphoroyloxy) ethyl methacrylate (OPEMA) units in a PIOP chain was 2.02.
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The synthetic conditions and characterizations of the hydrogels are summarized in Table 3. Figure 5 shows macroscopic pictures of the swollen hydrogels prepared in this study. The hydrogels (G1, G2, and G3) shown in picture a) were prepared without porogen salts. When the crosslinking density is low, the hydrogels have a highly stretched network, which was experimentally observed as a large transparent appearance. With an increase in the composition of PIOP, the size of the hydrogels decreased and the transparency became poor because of the close distance of the PIOP molecules. Picture b) shows porous hydrogels (G1A, G2A, and G3A) prepared with the largest porogen salts (ϕ = 300-500 µm). The effect of PIOP composition on the macroscopic form was similarly observed as in picture a). This result indicates that PIOP works as a macromolecular crosslinking reagent in the preparation of hydrogels. Many small bubbles are observed in the hydrogels prepared with porogen salts. Macroscopic observation clarifies the difference in the inner structure between G1 and G1A.
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Figure 5.
Macroscopic pictures of swollen hydrogels. a) Hydrogels without porogen salts (G1, G2, and G3) b) Hydrogels with porogen salts (G1A, G2A, and G3A) after 24 h equilibration in water. (Reproduced from Wachiralarpphaithoon et al., (2007)\n\t\t\t\t\t\t\tBiomaterials, Vol. 28, No. 6, pp. 984-993, Copyright (2007), with permission from Elsevier)
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Figure 6.
Enzymatic degradation as a function of time for hydrogel G1A in ALP aqueous solution at 37°C; [ALP]= 0 U/L (□), 72.5 U/L (∆), 220 U/L (○). Each point represents the average of three samples. (Reproduced from Wachiralarpphaithoon et al., (2007)\n\t\t\t\t\t\t\tBiomaterials, Vol. 28, No. 6, pp. 984-993, Copyright (2007), with permission from Elsevier)
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Alkaline phosphatase (ALP) is an important enzyme produced in bone and liver cells. It catalyzes the hydrolysis of phosphate groups from monophosphate ester substrates mostly found in an alkaline state with a pH of 9 (Coburn et al., 1998). Although Zhao and co-workers reported that synthetic polyphosphoesters and polyphosphoesters are enzymatically degradable (Zhao et al., 2003), the process was not described in detail. The concentration of ALP for the degradation study was adjusted to 72.5 and 220 U/L, which is the concentration in healthy adults and children, respectively (Takeshita et al., 2004; Rafan et al., 2000). Figure 6 is an enzymatic degradation profile of G1A hydrogels by changing the concentration of ALP. G1A took about 100 days to reach complete dissolution at pH 9.0. The degradation was accelerated with a higher concentration of ALP; G1A completely degraded after 60 days in 220 U/L of ALP. The degradation period was shortened with an increase in the concentration of the enzyme. The digestion of a hydrogel might be regulated by varying the density of cells secreting an enzyme in the hydrogel.
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MC3T3-E1 is a clonal osteogenic cell line derived from neonatal mouse calvaria. The cells are well characterized and provide a homogeneous source of osteoblastic cells for study. They were encapsulated in various biomaterial networks and remained viable (Burdick et al., 2005). MC3T3-E1 cells express high levels of alkaline phosphatase and differentiate into osteoblasts that can form calcified bone tissue in vitro (Choi et al., 1996). The response of MC3T3-E1 cells to many growth factors and hormones mimics that of primary cultures of rodent osteoblastic cells.
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Figure 7.
Kinetics of MC3T3-E1 cell proliferation in hydrogels. (○) G1A, (∆) G2A, (□) G3A with bFGF; (●) G1A, (▲) G2A, (■) G3A without bFGF. (Reproduced from Wachiralarpphaithoon et al., (2007)\n\t\t\t\t\t\t\tBiomaterials, Vol. 28, No. 6, pp. 984-993, Copyright (2007), with permission from Elsevier)
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\n\t\t\t\t\tFigure 7 shows the time-dependent concentration of the DNA produced from the MC3T3-E1 cells in porous hydrogels. The concentration increment of DNA corresponds to the proliferation of cells in a hydrogel. Under every sample condition, the amount of DNA significantly increased (p < 0.05) with increased cultivation time. After culture for 168 h, the amount of DNA collected was significantly higher from G3A (p = 0.036) in comparison to G1A. Therefore, the density of PIOP influenced cell proliferation. When the bFGF was incorporated into a hydrogel, the rate of cell proliferation relatively increased with an increase in the concentration of PIOP (p = 0.017 and p = 0.107 G1A vs. G3A after culture for 96 h and 168 h, respectively). While MPC polymer provides a suitable condition for maintaining cell viability, this polymer is not effective for inducing cell adhesion on the surface (Wachiralarpphaithoon et al., 2007). Polyphosphoester might induce cell adhesion and proliferation in a hydrogel. Wang and co-workers have recently reported that poly(ethylene glycol) (PEG) hydrogel having a phosphoester linkage promotes gene expression of bone-specific markers and secretion of alkaline phosphatase, osteocalcin, and osteonectin protein from marrow-derived mesenchymal stem cells (Wang et al., 2005).
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\n\t\t
\n\t\t
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3. Thermoresponsive polyphosphoesters
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Thermoresponsive polymers are widely studied in both research and technology because of their versatility in many fields. Recent trends in the application of polymer materials are drug delivery (Kikuchi & Okano, 2002), separation of bioactive molecules (Kobayashi et al., 2003), and tissue engineering (Kikuchi & Okano, 2005).\n\t\t\t\tN-Substituted acrylamide polymers have been found to have a phase separation characteristic with changes occurring in their properties upon heating above a certain lower critical solution temperature (LCST) (Monji et al., 1994; Yamazaki et al., 1999; Idziak et al., 1999). In particular, N-isopropyl acrylamide (NIPAAm) is one of the best monomers for accomplishing this; the homopolymer has LCST at 32°C in aqueous solution (Heskins et al., 1968). Although NIPAAm is a robust monomer for obtaining thermoresponsive polymer materials such as stimuli-responsive surfaces, particles, and hydrogels, the polymers are not biodegradable.
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Besides the stimuli-responsive nature, biodegradability and biocompatibility are important characteristics for polymeric materials used in biomedical fields. While the thermoresponsivity of some biodegradable polymers such as aliphatic polyester block copolymers or polypeptides was recently advanced (Fujiwara et al., 2001; Kim et al., 2004; Tachibana et al., 2003; Shimokuri et al., 2006), the molecular design and synthetic processes of thermoresponsive biodegradable polymers are still limited.
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3.1. Thermoresponsivity of polyphosphoesters
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In current research, thermoresponsive polyphosphoesters are now being synthesized with simple copolymerization of cyclic phosphoester compounds and their properties are being investigated (Iwasaki et al., 2007). Poly(IPP-co-EP) (PIxEy (Scheme 4); x:IPP (mol%), y: EP (mol%)) was synthesized by ring-opening polymerization using TIBA as an initiator. The range of weight-averaged molecular weights was 1.2 x 104 to 1.5 x 104 g/mol (GPC analysis).
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Scheme 4.
Synthetic route of PIxEy (Reproduced from Iwasaki et al., (2007)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138, Copyright (2007), with permission from the American Chemical Society)
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\n\t\t\t\t\tFigure 8 shows the LCST-type phase separation of PI24E76 aqueous solution. From the optical microscopic image, it is clear that the polymer solution was separated at the liquid-liquid phase above the cloud point. This appears to be coacervation. After several hours, the turbid solution spontaneously separated into two phases. The cloud point could be controlled by the ratio of IPP and EP, that is, it decreased with an increase in the molar fraction of hydrophobic IPP.
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Figure 8.
LCST-type phase separation of polyphosphoester aqueous solution. (a) 1%- PI24E76 aqueous solution at 20 and 40°C. (b) Optical micrograph of 1%-PI24E76 aqueous solution at 40°C. (Reproduced from Iwasaki et al., (2007)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138,Copyright (2007), with permission from the American Chemical Society)]
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Figure 9.
Effect of molecular fraction of IPP on LCST of PIxEy (Reproduced from Iwasaki et al., (2007)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138. Copyright (2007), with permission from the American Chemical Society)
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\n\t\t\t\t\tFigure 9 shows the effect of the composition of the monomer unit on the LCST of the copolymers. The LCST of poly(EP) (PEP) was 38°C and it linearly decreased with an increase in the ratio of IPP. IPP is relatively hydrophobic; the homopolymer of IPP is not soluble in water above 5°C. Dehydration of the polymer then preferably occurred with the addition of the hydrophobic IPP unit. It is reported that the LCST of thermoresponsive polymers can be controlled by the ratio of the hydrophobic and hydrophilic units (Takei et al., 1993; Tachibana et al., 2003). Thermoresponsivity under physiological conditions is effective for drug delivery or tissue engineering applications (Okuyama et al., 1993; Nishida et al., 2004). The thermoresponsivity of polyphosphoesters can also be observed under physiological temperatures. Thus, the polymers are applicable in the biomedical field.
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The effect of NaCl concentration on the cloud point on PEP and PI24E76 is shown in Figure 10. The cloud point of the polymer solution decreased with an increase in the concentration of NaCl in aqueous media. Under physiological conditions ([NaCl] = 100 mM), the cloud point of PEP and PI24E76 was 28 and 26°C, respectively. The solution property of nonionic polymer in water is sensitively influenced by the addition of salt because salt can alter polymer-water interaction (Foss et al., 1992).
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\n\t\t\t\t\tFigure 11 shows the dependence of the cloud point of PI24E76 on polymer concentration in distilled water. The cloud point decreased with an increase in polymer concentration. Furthermore, the change in the transmittance of the polymer solution was more abrupt at a higher concentration. The effect of polymer concentration on phase separation temperature was also observed on poly(acryl amide) derivatives (Miyazaki & Kataoka, 1996). In their report, coacervate droplets could be condensed with centrifugation; the polymer concentration of the coacervate phase was much greater than that of the homogeneous solution.
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Figure 10.
Effect of NaCl concentration ([NaCl]) on cloud point of polyphosphoester aqueous solution. (●) PE, (○) PI24E76, [Polymer] = 1.0 wt%.
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Figure 11.
Effect of polymer concentration on cloud point of PI24E76 aqueous solution. [Polymer] = 1.0 (♦), 0.75 (●), 0. 5 (▲), 0.25 (■), and 0.1 wt% (x).
Spin-lattice relaxation time (T\n\t\t\t\t\t\t\t1) and spin-spin relaxation time (T\n\t\t\t\t\t\t\t2) of proton in PI24E76.
\n\t\t\t\t
To understand the molecular phenomenon for creating coacervates, we measured T\n\t\t\t\t\t1 and T\n\t\t\t\t\t2 of the protons in the main and side chains of PI24E76. Table 4 summarizes the typical data for relaxation times. It can be considered that a polymer in solution behaves as a liquid molecule with high mobility (Mao et al., 2000). As shown in Table 4, T\n\t\t\t\t\t1 and T\n\t\t\t\t\t2 of every proton contained in the main and side chains of PI24E76 increase as the temperature increases. Furthermore, a significant change of these relaxation times at the cloud point of PI24E76 was not observed. T\n\t\t\t\t\t2 of the protons is mostly influenced by the dipole-dipole interaction of nuclear spin. The shorter the distance between protons, the slower the motion of the polymer chains and the stronger the interaction of the proton-proton dipolar coupling; thus the smaller T\n\t\t\t\t\t2. The experimental results indicated that the mobility of the polymer thermodynamically increased with an increase in temperature regardless of the phase separation.
\n\t\t\t\t
Figure 12.
Condensation of hydrophobic compound (Nile Red) from aqueous media. a) 150 mM NaCl aqueous solution, b) 150 mM NaCl aqueous solution containing 1-wt% PI24E76. [Nile Red] = 5 µg/mL.
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The relaxation times of the protons of associated trigger groups normally decrease because of a decrease in mobility (Hsu et al., 2005). However, the results did not show this. In the coacervate phase with enriched polymers, solvent remained above the cloud point. Then, the polymers might loosely associate and their mobility was not reduced with an increase in temperature. While the mobility of the polymers in the coacervate phase was clarified, further study will be needed to show the molecular mechanism of coacervation.
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We demonstrated the separation of hydrophobic molecules with thermoresponsive polyphosphoesters from aqueous media. Nile Red was used as a model compound; its solubility in water is very low. Nile Red dissolved in acetone was added to Dulbecco’s phosphate buffered saline (PBS, calcium chloride- and magnesium chloride-free, Sigma). Polyphosphoester was then immediately introduced into the solution. Both PBS and that containing the polymer appear homogeneous before heating. When the solutions were incubated at 40°C, significant differences in solution behavior were observed, as shown in Figure 12. At 40°C, the polymer solution became turbid and then separated into two phases. Nile Red selectively condensed at the bottom layer, which contains the concentrated polymers. In contrast, the aggregation of Nile Red was observed in PBS at 40°C because the acetone evaporated and the Nile Red could not then disperse in the aqueous solution. After a decrease in temperature back to 4°C, the polymer solution appeared clear and homogeneous, but the aggregation of Nile Red remained in the PBS. The polyphosphoesters interact with hydrophobic Nile Red and help its dispersion. Furthermore, the precipitation of Nile Red was not observed even after the polymer solution was diluted 100 times with PBS. By using polyphosphoesters, we were able to improve the solubility of hydrophobic molecules in aqueous media and separate them with temperature increments.
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Wang and co-workers also observed the thermoresponsivity of polyphosphoesters. They have synthesized well-defined block copolymers of poly(ethylene glycol) and polyphosphoester (Wang et al., 2009). Block copolymers can form core-shell type polymeric micelles in an aqueous medium with the effect of temperature caused by self-association of the polyphosphoester block. Although it is clear that polyphosphoester is the new candidate thermoresponsive polymer, its properties have only been partially evaluated. The effect of molecular weight on the cloud point of PIPPn (Scheme 1) has not been discussed. Figure 13 shows the dependence of the phase separation temperature of PIPP in phosphate buffered saline (PBS) on molecular weight.
\n\t\t\t\t
Figure 13.
Effect of molecular weight on cloud point of poly(2-isopropoxy-2-oxo-1,3,2-dioxaphospholane) (PIPP) (1 wt %) in PBS. (●) PIPP50(DBU), (■) PIPP48(TBD), (♦) PIPP32(DBU), (▲) PIPP13(DBU). (Reproduced from Iwasaki et al., (2010)\n\t\t\t\t\t\t\tMacromolecules, Vol. 40, No. 23, pp. 8136-8138, Copyright (2010), with permission from the American Chemical Society)
\n\t\t\t\t
The cloud point of the polymer solution decreases with an increase in the molecular weight of PIPP. The result indicates that the type of organocatalyst does not influence the phase separation temperature. The phase separation temperature of polyphosphoesters is influenced by the chemical structure of the side chains, the concentration, and the ion strength of the aqueous media. In our previous report, PIPP that was synthesized using TIBA as an initiator was not soluble in water even when the molecular weight was less than 1.0 x 104 (Iwasaki & Akiyoshi, 2004). An uncontrolled reaction might occur when a metallic catalyst was used. Wang reported that long-term polymerization of cyclic phosphoesters with Sn(Oct)2 makes some branch structures with high conversion rates (Xiao et al., 2006). In addition, some side reactions might occur in ring-opening polymerization of five-membered cyclic phosphoesters at high temperature (Liu et al., 2009). Furthermore, the molecular weight distribution of polyphosphoesters synthesized with an organocatalyst was significantly narrow compared with polymers that used metallic catalysts. The advantages of using organocatalysts can be observed on the synthesis of well-defined polymers with high conversion rates.
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\n\t\t\t\t
3.2. Polyphosphoester macroinitiators
\n\t\t\t\t
Thermoresponsive polymers have great potential in bioscientific applications (Alarcon et al., 2005; Klouda et al., 2008). In particular, the selective delivery of drugs to target sites through hyperthermia could be performed (Chikoti et al., 2002). However, heat treatment might induce adverse effects on normal tissue and limitations remain in terms of selectivity. A polymer that can change its thermoresponsivity after contact with esterase has been synthesized. As shown in Scheme 5, polyphosphoesters bearing benzyl groups were synthesized. The synthetic results are listed in Table 5. The polymerization ability of BP and EP was similar. The 1H NMR spectra of the polymers at each reaction step are summarized in Figure 14. After treatment with Pd/C in formic acid, a signal caused by the aromatic group at around 7.2 ppm disappeared. Deprotection of benzyl groups from PEB was completely accomplished and PEH was obtained. Then, PEH reacted with acetoxymethyl bromide in the presence of ethyldiisopropylamine. The 1H NMR spectrum of PEHA clarified that the acetoxymethyl group was introduced at the deprotected position. No decrease in molecular weight was observed. No polymer degradation occurred during the introduction of the AM groups.
\n\t\t\t\t
Scheme 5.
Synthetic route of polyphosphoester bearing acetoxymethyl groups
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The enzymatic digestion of acetoxymethyl esters from PEHA was evaluated in contact with porcine liver esterase for a specific time. Figure 15 shows the time dependence of the relative fraction of the acetoxymethyl groups on the EP units. The data are represented as the mean from 4 samples. When the enzyme was treated with PEHA, the decrease in the fraction of AM groups was dramatic compared to that soaked in PBS for 24 h. The fraction then gradually decreased over time. Esterase activity might influence this data. Geurtsen and co-worker reported that the activity of porcine liver esterase decreased during the first 24 h to approximately 40% and then remained constant for up to 6 days (Geurtsen et al., 1999). Even in synthetic polymer systems, the effect of esterase has been observed. The AM groups spontaneously degraded in PBS. The degradation rate at the early stage was much slower than that of the esterase treatment.
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\n\t\t\t\t\t\t
\n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t
Polymer
\n\t\t\t\t\t\t\t
Molar fraction
\n\t\t\t\t\t\t\t
\n\t\t\t\t\t\t\t\tM\n\t\t\t\t\t\t\t\tn x 10-3\n\t\t\t\t\t\t\t
Synthetic results of polyphosphoester bearing acetoxymethyl groups
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Figure 14.
NMR spectra of polyphosphoester bearing acetoxymethyl ester groups and the prepolymers.
\n\t\t\t\t
\n\t\t\t\t\tFigure 16 shows the change in the number-averaged molecular weight (M\n\t\t\t\t\tn) of PEHA incubated in PBS and that containing esterase. The decrease in molecular weight of PEHA was remarkable when the polymer was in contact with esterase. Digestion of the main chain was also accelerated with the esterase treatment.
\n\t\t\t\t
Figure 15.
Change in unit mole fraction of acetoxymethyl ester group of PEHA in contact with porcine liver esterase. (●) in PBS, (○) in esterase solution [Esterase] = 40 U/mL.
\n\t\t\t\t
The thermoresponsivity of PEHA before and after contact with protease is shown in Figure 17. The PEHA/PBS showed LCST-type liquid-liquid phase separation and the cloud point was 40°C. In both PBS and that with esterase, the temperature of the phase separation increased with an increase in incubation time. In particular, the PEHA treated with esterase for 24 h did not have a cloud point between 20 and 65°C. The degree of AM groups on the polymer influenced its thermoresponsivity. That is, the phase separation phenomena could be controlled by acetoxymethylation of the polyphosphoesters. In addition, PEH, the polymer before acetoxymethylation, did not show any LCST-type liquid-liquid phase separation (data not shown). The influence of the change in molecular weight of PEHA with esterase treatment should also be of concern. While the cloud point of PEHA synthesized in this study was not in physiological conditions (>40°C), it could be adjusted by introducing more hydrophobic units into the polymer as described in previous literature (Iwasaki et al., 2004). Because the block copolymers composed of polyphosphoesters and poly(ethylene glycol) form a micelle structure above phase separation temperature (Wang et al., 2009), PEHA will work as building blocks for making enzyme-responsive micelles.
\n\t\t\t\t
Figure 16.
Change in number-averaged molecular weight (Mn) of PEHA in contact with porcine liver esterase. (●) in PBS, (○) in esterase solution [Esterase] = 40 U/mL.
\n\t\t\t\t
Figure 17.
Thermoresponsivity of PEHA in PBS before and after incubation with porcine liver esterase for 6 and 24 h. (●) 0, (▲) 6, and (□) 24 h in PBS; (∆) 6 h and (□) 24 h in esterase solution.
\n\t\t\t\t
The AM group is widely used for prodrugs and for fluorescence probes for cell imaging (Hecher et al., 2008; Takakusa et al., 2003). This group effectively induces cell membrane penetration and is rapidly cleaved intracellularly (Shultz et al., 1993; Yogo et al., 2004). Figure 18 is a fluorescence micrograph of HeLa cells in contact with Nile Red for 60 min with or without PEHA. The localization of Nile Red into the cells was improved by the presence of PEHA. At this concentration of PHEA, the polymer does not have a cloud point around 37°C. The solubilization capacity for hydrophobic molecules and the amphiphilic nature of the polymer might be improved by the cytoplasmic penetration of Nile Red. Although the mechanism of delivery of Nile Red into cells has not been fully clarified, the polyphosphoester bearing AM groups has the potential to induce penetration of hydrophobic drugs through the cell membrane.
\n\t\t\t\t
To understand the interaction of PEHA and the cell membrane, we investigated the cytotoxicity of PEHA using Chinese hamster fibroblasts (V79), as described in a previous report (Iwasaki et al., 2004). There was no adverse effect of PEHA on cell viability when the PEHA concentration was below 0.01 g/dL (see supporting data). On the other hand, the cytotoxicity of PEHA was observed when the concentration was more than 0.1 g/dL. From the nature of this cytotoxicity test, it can be assumed that a high concentration of PEHA might damage the cell membrane. That is, that PHEA has an affinity for cell membrane.
\n\t\t\t\t
Figure 18.
Fluorescence micrographs of HeLa cells in contact with Nile Red in culture medium. a) Nile Red, b) Nile Red with PEHA. [PEHA] = 0.0025 mg/mL, [Nile Red] = 0.0125 µg/mL.
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4. Conclusion
\n\t\t\t
This chapter described current studies of new methods of syntheses and the characteristics of polyphosphoesters. Polymerization with a narrow molecular weight distribution is important to obtain the reproducible properties of polymers. In addition, the functionalization of the end or side groups of the polymers results in producing various types of polymer materials. The robustness of polyphosphoesters as biomedical materials has been clarified during the past decade (Zhao et al., 1003; Wang et al., 2009). However, the molecular and material designs of polyphosphoesters for biomedical applications are still limited. Polyphosphoesters have been explored as biomimetic to nucleic and teichoic acids. The study of the biological activity of polyphosphoesters will prove to be interesting.
\n\t\t\t
As one of the unique properties of polyphosphoesters, LCST-type liquid-liquid phase separation of polyphosphoesters in aqueous media was introduced with a difference in the structure of their side chains. The aqueous solution of the polymers bearing alkyl groups became turbid with increments in temperature. From microscopic observation, liquid-liquid phase separation was observed in the turbid solution. The cloud points of the polymer solutions were influenced by polymer concentration, copolymerization ratio, and NaCl concentration. In addition, the copolymer effectively improved the solubility of the hydrophobic molecules in an aqueous medium and enabled separation of the molecules from the solution with increments in temperature.
\n\t\t\t
Furthermore, thermoresponsive polyphosphoesters bearing AM groups as side chains were demonstrated as enzyme-responsive polymers. The thermoresponsivity of polymers in aqueous solution depended on the concentration of AM units and their molecular weight. Cleavage of the AM units and degradation of the polymer chain were accelerated with esterase treatment. The solubility of hydrophobic molecules and localization of the molecules into living cells were also improved by the synthetic polymers. To use polyphosphoesters bearing AM groups as drug carriers, further molecular design to achieve self-assembly, stealth, and targeting characteristics will be needed. However, the newly designed structure is interesting as a basic motif for applications.
\n\t\t
\n\t
Acknowledgments
\n\t\t\t
Some activities described in this chapter were supported by a Grant-in-Aid for Scientific Research on Innovative Areas "Molecular Soft-Interface Science" (#21106520) and Young Scientists (A) (#21680043) from the Ministry of Education, Culture, Sports, Science and Technology of Japan. The author is grateful to Dr. Shin-ichi Yusa (University of Hyogo), Ms. Etsuko Yamaguchi (Kansai University), and Mr. Takashi Kawakita (Kansai University) for their assistance in the synthesis and characterization of the polyphosphoesters.
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\n',keywords:",",chapterPDFUrl:"https://cdn.intechopen.com/pdfs/17640.pdf",chapterXML:"https://mts.intechopen.com/source/xml/17640.xml",downloadPdfUrl:"/chapter/pdf-download/17640",previewPdfUrl:"/chapter/pdf-preview/17640",totalDownloads:3007,totalViews:189,totalCrossrefCites:0,totalDimensionsCites:3,hasAltmetrics:0,dateSubmitted:"October 28th 2010",dateReviewed:"April 10th 2011",datePrePublished:null,datePublished:"August 1st 2011",dateFinished:null,readingETA:"0",abstract:null,reviewType:"peer-reviewed",bibtexUrl:"/chapter/bibtex/17640",risUrl:"/chapter/ris/17640",book:{slug:"biomedical-engineering-frontiers-and-challenges"},signatures:"Yasuhiko Iwasaki",authors:[{id:"31795",title:"Dr.",name:"Yasuhiko",middleName:null,surname:"Iwasaki",fullName:"Yasuhiko Iwasaki",slug:"yasuhiko-iwasaki",email:"yasu.bmt@kansai-u.ac.jp",position:null,institution:null}],sections:[{id:"sec_1",title:"1. Introduction ",level:"1"},{id:"sec_2",title:"2. Synthesis of well-defied polyphosphoesters and incorporation of functional groups into polymers",level:"1"},{id:"sec_2_2",title:"2.1. Synthesis of polyphosphoesters using organocatalysts",level:"2"},{id:"sec_3_2",title:"2.2. Polyphosphoester macroinitiators",level:"2"},{id:"sec_4_2",title:"2.3. Polyphosphoester macrocrosslinkers",level:"2"},{id:"sec_6",title:"3. Thermoresponsive polyphosphoesters",level:"1"},{id:"sec_6_2",title:"3.1. Thermoresponsivity of polyphosphoesters",level:"2"},{id:"sec_7_2",title:"3.2. Polyphosphoester macroinitiators",level:"2"},{id:"sec_9",title:"4. Conclusion",level:"1"},{id:"sec_10",title:"Acknowledgments",level:"1"}],chapterReferences:[{id:"B1",body:'\n\t\t\t\t\n\t\t\t\t\tAlarcon, C.D.H.; Pennadam, S.; Alexander, C. (2005). Stimuli Responsive Polymers for Biomedical Applications. 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Biomacromolecules, Vol. 10, No. 1, (January 2009), pp. 66-73, ISSN 1526-4602\n\t\t\t'},{id:"B58",body:'\n\t\t\t\t\n\t\t\t\t\tWang, Y.-C.; Yuan, Y.-Y.; Du, J.-Z.; Yang, X.-Z. ; Wang, J. (2009). Recent Progress in Polyphosphoesters: From Controlled Synthesis to Biomedical Applications. Macromolecular Bioscience, Vol. 9, No. 12, (December 2009), pp. 1154-1164, ISSN 1616-5195\n\t\t\t'},{id:"B59",body:'\n\t\t\t\t\n\t\t\t\t\tWen, J. & Zhuo, R.X. (1998). Enzyme-Catalyzed Ring-Opening Polymerization of Ethylene Isopropyl Phosphate. Macromolecular Rapid Communications, Vol. 19, No. 12, (December 1998), pp. 641-642, ISSN 1521-3927\n\t\t\t'},{id:"B60",body:'\n\t\t\t\t\n\t\t\t\t\tXiao, C.-S.; Wang, Y.-C.; Du, J.-Z.; Chen, X.-S.; Wang, J. (2006). Kinetics and Mechanism of 2-Ethoxy-2-oxo-1,3,2-dioxaphospholane Polymerization Initiated by Stannous Octoate. Macromolecules, Vol. 39, No. 20, (September 2006), pp. 6825-6831, ISSN 1520-5835\n\t\t\t'},{id:"B61",body:'\n\t\t\t\t\n\t\t\t\t\tYamazaki, A.; Winnik, F.M.; Cornelius, R.M.; Brash, J.L. (1999). Modification of Liposomes with N-Substituted Polyacrylamides: Identification of Proteins Adsorbed from Plasma. Biochimica et Biophysica Acta (BBA)- Biomembranes, Vol. 1421, No. 1, (September 1999), pp. 103-115, ISSN 0005-2736\n\t\t\t'},{id:"B62",body:'\n\t\t\t\t\n\t\t\t\t\tYogo, T.; Kikuchi, K.; Inoue, T.; Hirose, K.; Iino, M.; Nagano, T. (2004). Modification of Intracellular Ca2+ Dynamics by Laser Inactivation of Inositol 1,4,5-Trisphosphate Receptor Using Membrane-Permeant Probes. Chemistry and Biology, Vol. 11, No. 8, (August 2004), pp. 1053-1058, ISSN 1879-1301\n\t\t\t'},{id:"B63",body:'\n\t\t\t\t\n\t\t\t\t\tZhao, Z.; Wang, J.; Mao, H.Q.; Leong, K.W. (2003). Polyphosphoesters in Drug and Gene Delivery. Advanced Drug Delivery Reviews, Vol. 55, No. 4, (April 2003), pp. 483-499\n\t\t\t'}],footnotes:[{id:"fn1",explanation:"The number after PMPC is degree of MPC polymerization in each graft chain."}],contributors:[{corresp:null,contributorFullName:"Yasuhiko Iwasaki",address:null,affiliation:'
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1. Introduction
In a shallow water body, beach changes may take place owing to wind waves. In a narrow water body with a large aspect ratio, the angle of wind waves relative to the direction normal to the shoreline may exceed 45°, and the shoreline may become unstable because the fetch distance in the direction of the principal axis of the water body is sufficiently large for waves with significant energy to be generated [1, 2]. Therefore, cuspate forelands that develop from both shores of a narrow water body connect with each other, resulting in the segmentation of the water body into smaller rounded lakes [3, 4]. For example, Figure 1 shows the segmentation of a lagoon facing the Chukchi Sea in Russia [3, 4]. In this example, five elliptic lakes can be observed as a result of segmentation, and their axes are parallel to each other. Figure 2 shows an enlarged satellite image of the rectangular area in Figure 1, and in this image, lake segmentation at a primitive stage can be seen with the alternate development of cuspate forelands. Regarding these phenomena, the division and reduction of the fetch distance owing to the formation of a large shoreline protrusion associated with shoreline instability under high-wave-angle conditions and the resulting change in the wave field are key factors. Ashton et al. [4] predicted that the forelands formed along the shoreline connect with each other, resulting in the segmentation of the water body into smaller rounded lakes. Uda et al. [5] predicted the three-dimensional (3-D) segmentation of a shallow rectangular water body using the BG model (a model for predicting 3-D beach changes based on Bagnold’s concept) [6]. Uda et al. studied the emergence and mergence of small lakes and their segmentation using the same model [7], assuming that the wind blew from all directions between 0 and 360° with the same probability of occurrence and intensity, that is, a circular distribution of the probability. The segmentation into elliptic shapes, as shown in Figure 1, was not predicted in their study. It may be accomplished, assuming that the probability of occurrence of the wind direction is given by an elliptic distribution, similarly to the case of oriented lakes [8]. In this study, the segmentation of a rectangular water body was predicted, given a circular or elliptic distribution of the probability of occurrence of the wind direction.
Figure 1.
Example of segmentation of slender water body: Lagoons facing Chukchi Sea [3, 4].
Figure 2.
Enlarged satellite image of rectangular area in Figure 1.
In the coastal area, the segmentation of a shallow water body with a triangular or crescent shape can also be observed. To study the mechanism of segmentation of such a water body, several examples of segmentation together with the development of sand spits along the lakeshore were examined in Lagoa de Mangueira in Brazil, Lake Saroma and Lake Kitaura in Japan. Then, the BG model was used to investigate the segmentation of a shallow water body with a triangular or crescent shape, and 3-D beach changes during the segmentation of a shallow water body into small lakes were predicted.
When wind waves are incident to the lakeshore in a closed water body with a rocky or sandy island, topographic changes may occur on the lee of the island because of the wave-sheltering effect. Since a rocky island is fixed at a location in a closed water body, the wave-sheltering effect of the island is constant with time, and the lakeshore converges to a certain stable form after the wave action for a sufficiently long time. When a sandy island is located in a closed water body, however, the island itself can deform owing to the action of wind waves, resulting in the successive change in wave field. Thus, more complicated lakeshore changes will occur. Here, Lake Balkhash located in Kazakhstan [9] was selected as an example, and the BG model was used for predicting lakeshore changes when a rocky or sandy island exists in a circular lake.
2. Examples of cuspate forelands in lake
2.1. Lakeshore in Lagoa de Mangueira
Figure 3 shows an example of segmentation and the development of sand spits along the lakeshore of Lagoa de Mangueira (location: 33°09′59”S, 52°49′32”W) in Brazil [7]. The crescent lake is 100 km long and 10 km wide at the center of the lake. Many cuspate forelands have developed along the lakeshore and, in particular, the intervals of the cuspate forelands formed on the west shore become short near the south end of the lake. On the other hand, sand spits with similar shapes and cuspate forelands have developed along the east and west shores, respectively, in the north part of the lake. This is a typical example of segmentation and the development of sand spits in a crescent lake.
Figure 3.
Segmentation and development of sand spits along lakeshore of Lagoa de Mangueira in Brazil [7].
2.2. Lakeshore in Lake Saroma
Figure 4 shows a satellite image of an abandoned inlet located at the east end of Lake Saroma in Hokkaido, Japan (Location: 44°08′03”N, 143°59′04″E) [10]. This water body has a triangular shape, and segmentation of a water body can be seen near the east end. When enlarging the rectangular area in the satellite image of Figures 4 and 5 is obtained. For the wind rose in Lake Saroma, the predominant wind direction is WNW, resulting in the eastward development of sand spits. On the south shore is Tofutsu fishing port, as shown in Figure 5. East of this fishing port, the width of the water body gradually decreases, and sand spits A-E develop together with pairs of sand spits A’ and E’. Of these sand spits, sand spits A and A’ are the largest and divide the water body into two. In the vicinity of sand spit A’, wind waves cannot be generated in the presence of the westerly wind, resulting in no development of sand spits. However, east of sand spit A’, wind waves can develop, and the size of the sand spits increases eastward in the order of sand spits B, C, and D.
Figure 4.
Study area in eastern Lake Saroma [10].
Figure 5.
Enlarged satellite image of rectangular area in Figure 4, and sand spits A-E and E’ [10].
2.3. Lakeshore in Lake Kitaura
Lake Kitaura located in Ibaraki Prefecture is a shallow lake with an area of 35.2 km2 and 25 km length in the north-south direction, as shown in Figure 6. The formation of cuspate forelands in this lake was discussed in [5], and here we refer this results. This lake is located in the lowland surrounded by Kashima and Namegata tablelands with elevations of 40 and 30 m on the east and west sides, respectively. Thus, wind waves can be generated without a significant sheltering effect by hills or mountains. Because the direction of the principal axis of Lake Kitaura is N18°W, the predominant wind of NNE blows at an angle of 40.5° clockwise relative to the direction of the principal axis. Because of this oblique wind direction, wind waves are incident at a large incidence angle to the shoreline, resulting in the formation of the protruding shoreline on the west shore. In particular, an enlarged satellite image of two subareas,a and b, in Figure 6 is shown in Figure 7. In subarea a, cuspate forelands and the ridges develop out of phase, and this condition is very similar to that in the lagoon facing the Chukchi Sea, as shown in Figure 2. Similarly, the cuspate forelands on both shores extend out of phase in subarea b. This shows a typical example of segmentation and the development of sand spits in a triangular lake.
Figure 6.
Cuspate forelands developed along lakeshore of Lake Kitaura in Japan [5].
Figure 7.
Enlarged satellite images of areas a and b in Lake Kitaura [5].
2.4. Lake Balkhash
Lake Balkhash has 450 and 200 km lengths in the E-W and S-N directions, respectively (Figure 8). Figure 9 shows an enlarged satellite image of the rectangular area in Figure 8. Island A is located at a location of 46°34′53.99”N and 78°50′17.47″E at the central part of the lake near the east end, and a cuspate foreland of 14 km length extends between island A and the lakeshore. On the shore opposite to island A, a triangular cuspate foreland B is formed with a barrier island. The sand bar extending northwestward from Island A is symmetric with respect to the centerline of the cuspate foreland, and the length of the sand bar is longer than the width of the island. From this, it is inferred that the cuspate foreland extended from the land to Island A by the sand supply from Island A and the land, and connected to Island A.
Figure 8.
Satellite image of Lake Balkhash in Kazakhstan.
Figure 9.
Enlarged satellite image of Lake Balkhash.
3. Model for predicting lakeshore changes
For the calculation of the segmentation of a rectangular water body, the BG model employed for the calculation of oriented lakes [8] was used. Given a local fetch distance F at a given point (g is the acceleration due to gravity and U is the wind velocity), the significant wave height H1/3 was calculated using Wilson’s formula [11, 12].
H1/3=fF,U=0.301−1+0.004gF/U21/2-2U2/gE1
In this calculation, a coordinate system (xw, yw) was set corresponding to the wave direction instead of a fixed coordinate system (x, y) for the calculation of beach changes with the rectangular calculation domain, ABCD, as shown in Figure 10, and the wave height was calculated in the rectangular domain A’B’C’D’ including the domain ABCD. Neglecting the wave refraction effect, waves were assumed to propagate in the same direction as the wind. The fetch distance F was added from upwind to downwind along the xw-axis using Eq. (2) when the xw-axis was divided by mesh intervals Δxw [13]. Here, the index i in Eq. (2a) is the mesh number along the xw-axis.
Fi+1=Fi+r∆xwE2a
r=1Z≤00Z>0E2b
Figure 10.
Selection of coordinate system (x, y) adopted for calculation of beach changes with rectangular calculation domain ABCD and another coordinate system (xw, yw) [13].
When a grid point was located on land and the downslope condition of dZ/dxw ≤ 0 was satisfied, the local fetch was reset as F = 0 (Eq. (3)).
Fi=0ifZ≥0anddZ/dxw≤0E3
When the grid point was located in the lake, F was recalculated. By this procedure, the wave height becomes 0 on the lee of the cuspate forelands, and the wave-sheltering effect alone can be evaluated.
For the sand transport equation, Eq. (4), which is expressed using the wave energy at the breaking point, was used [6].
q→=C0KsPtanβctanβcew→−cosα∇Z→−hc≤Z≤hRE4
P=εZECgbtanβwE5
tanβw=dZ/dxwtanβw≥0E6
Here, q→=(qx,qy) is the net sand transport flux, Z (x, y, t) is the seabed elevation with reference to the still water level (Z = 0), ∇Z→=(∂Z/∂x,∂Z/∂y) is the seabed slope vector, e→w the unit vector of the wave direction, α is the angle between the wave direction and the direction normal to the contour line, and |cosα| = |e→w⋅∇Z→|/|∇Z→|. tanβc is the equilibrium slope of sand, and Ks is the longshore and cross-shore sand transport coefficient. The P value in Eq. (5) is the wave dissipation ratio per unit area of the seabed and time between Z = −hc and hR, where sand movement occurs [6], and (ECg)b is the wave energy flux at the breaking point. xw is the coordinate in the direction of wave propagation, and tanβw is set to 0 when tanβw < 0 is satisfied. tanβw is the seabed slope measured in the direction of wave propagation. In the calculation, the local beach slope measured along the wave ray was used for the beach slope in Eq. (5), as shown in Eq. (6). hc is the depth of closure, and hR is the berm height. C₀ is the coefficient for transforming the immersed weight expression to the volumetric expression (C0=1/{(ρs−ρ)g(1−p)}; ρ is the seawater density, ρs is the specific gravity of sand, p is the sand porosity, g is the acceleration due to gravity), ε(Z) in Eq. (5) is the depth distribution of sand transport and is defined so as to satisfy Eq. (7); in this study, a uniform distribution was employed (Eq. (8)).
∫−hchRεZdZ=1E7
εZ=1/hc+hR−hc≤Z≤hRE8
If H1/3 is approximately equal to the breaker height Hb and γ is the ratio of the breaker height to water depth, the wave energy flux at the breaking point (ECg)b in Eq. (5) can be written as Eq. (9a).
ECgb=C1Hb52≈C1H1/352E9a
C1=ρgk1g/γk1=4.0042,γ=0.8E9b
When F and H1/3 are calculated using the coordinate system (xw, yw) according to the wave direction, the wave power P (Eq. (5)) can be calculated and assigned to each grid point on the coordinate system (xw, yw). The wave power P at each grid point in the calculation of beach changes was interpolated from this distribution of P. The mesh intervals (Δxw, Δyw) in the coordinate system (xw, yw) were taken to be the same as (Δx, Δy). Finally, the sand transport and continuity equations were solved on the x-y plane by the explicit finite-difference method using a staggered mesh scheme. In this study, the wind direction at each step in the calculation of beach changes was selected to be a value determined by random numbers so as to satisfy the probability distribution function of the occurrence of a certain wind direction, although the wind velocity was assumed to be constant.
In estimating the intensity of sand transport near the berm top and at the depth of closure, the intensity of sand transport was linearly reduced to 0 near the berm height or the depth of closure to prevent sand from being deposited in the zone higher than the berm height and the beach from being eroded in the zone deeper than the depth of closure [14].
4. Calculation conditions
Lakeshore changes in a rectangular water body with an aspect ratio of 5 owing to wind waves were first predicted when wind blew from all directions between 0 and 360° with the same probability of occurrence and intensity (Case 1) or blew at an angle of 45° relative to the principal axis of the rectangular water body with an elliptic probability of occurrence and intensity (Case 2), as shown in Figure 11 [13]. Then, lakeshore changes in triangle- and crescent-shaped shallow water bodies with a flatbed were predicted in Cases 3 and 4, respectively. In all cases, the water depth of the flatbed, the berm height, and the initial beach slope were set to 3 m, 1 m, and 1/20, respectively. Figure 12 shows the initial topography in each case. Random perturbations with the amplitude △Z = 0.1 m were added to the slope between Z = 1 and −3 m in the initial bathymetry. The wind velocity was 20 m/s. The calculation domain was discretized by △x = △y = 20 m with △t = 10 h. The depth distribution of sand transport was assumed to be a uniform distribution throughout the depth, and the equilibrium slope was 1/20. Table 1 shows the calculation conditions for Cases 1–4. The wind velocity of 20 m/s is the value at which a significant wave height of approximately 1 m, the same as the berm height, could be generated, given the fetch distance of 4.6 km, being the distance along the diagonal of the initial rectangular water body in Cases 1 and 2. In Cases 3 and 4, the wind velocity was also assumed to be 20 m/s, and wind was assumed to blow from all directions with the same probability and intensity.
Figure 11.
Probability distribution of occurrence of wind direction: (a) circular and (b) elliptic [13].
Figure 12.
Initial topographies in Cases 1–4.
Wind velocity
20 m/s
Berm height, hR
1 m
Depth of closure, hc
3 m
Equilibrium slope, tanβc
1/20
Coefficient of sand transport
Ks = 0.2
Calculation cases
Case 1: rectangular water body, circular probability distribution Case 2: rectangular water body, elliptic probability distribution Case 3: segmentation of a triangular water body Case 4: segmentation of a crescent-shaped water body Cases 5–8: topographic changes around an island located in a circular lake
Mesh size
Δx = Δy = 20 m
Time intervals
Δt = 10 h
Duration of calculation
106 h (105 steps) in Cases 1–4, 5 × 105 h (5 × 104 steps) in Cases 5–8
Boundary conditions
Shoreward and landward ends, qx = 0 Right and left boundaries, qy = 0
Table 1.
Calculation conditions.
In predicting lakeshore changes when a rocky or sandy island is located in a closed water body, four calculations were carried out, as shown in Figure 13. In each case, a circular lake with a radius of 1000 m and a solid bottom of a constant depth of 3 m was set for the calculation domain. In this circular lake, a rocky or sandy island with a radius of 200 m was set at locations deviating from the center of the lake. The foreshore slope of the lakeshore was assumed to be 1/20. In the present study, the incident angle of waves to the mean shoreline exceeds 45° at certain locations of the lakeshore, resulting in shoreline instability. Therefore, a small perturbation with the amplitude ΔZ = 0.1 m was added in the depth zone between Z = −3 and 1 m. In Cases 5 and 6, a rocky island was placed with its center deviating from the center of lake, and the wave-sheltering effect by the island was enhanced in Case 6, in which the island was set at a location closer to the lakeshore. In Cases 7 and 8, the arrangement of the island is the same as those in Cases 5 and 6, respectively, but the island is composed of sand. The other conditions are the same as those in Cases 1–4. Table 1 shows the calculation conditions for Cases 5–8.
Figure 13.
Arrangement of island in Cases 5–8.
5. Results
5.1. Segmentation of water body given circular distribution of probability (Case 1)
Figure 14 shows the calculation results for the segmentation of a slender, rectangular water body with a longshore length of 4.5 km, and a width of 0.9 km (aspect ratio = 5), assuming that the probability of occurrence of wind direction was given by a circular distribution [13]. When wind waves were incident to the lakeshore, several cuspate forelands with irregular shapes developed along the shoreline in the beginning. After 2 × 104 steps, the cuspate forelands merged with each other, resulting in a reduction in their number, and sand bars with a hound’s-tooth shape were formed. This development of cuspate forelands well explains the formation of the lakeshore, as shown in Figure 2. After 4 × 104 steps, sand bars extended to the opposite shores, and the water body was about to separate into two lakes, and then the water body had separated into two completely independent lakes. Finally, two completely rounded lakes were formed.
Figure 14.
Topographic changes in Case 1 under uniform distribution of occurrence of wind direction and intensity [13].
The distributions of the wave height and longshore sand transport alter in response to the wind direction at each time. The formation of cuspate forelands and rounded lakes over time, however, strongly depends on the mean (H1/3)5/2 flux averaged over a significantly long time [13]. Figure 15 shows the mean (H1/3)5/2 flux averaged over 103 steps at six stages between 1 × 103 and 1 × 105 steps. The arrows in the figure show the direction of the flux, and the color corresponds to the intensity of the flux. After 103 steps, outward flux was generated radially from the central part of the lake with a symmetric distribution, and the time-averaged flux at the central part was 0 because of the cancelation of the sum of the vectors. After 2 × 104 steps, the mean (H1/3)5/2 flux was equivalent on both sides of the central cuspate foreland, facilitating the development of the cuspate foreland. After 4 × 104 steps, the cuspate forelands had further developed, and the direction of the mean (H1/3)5/2 flux approached the direction normal to the shoreline. Finally, after 105 steps, its direction became normal to the shoreline of the rounded lake.
Figure 15.
Distribution of mean (H1/3)5/2 flux in Case 1 [13].
The mean sand transport flux after 4 × 104 and 5 × 104 steps in Case 1 can be drawn, as shown in Figure 16 [13]. Intensive sand transport flux occurred along the shoreline of a cuspate foreland at the central part of the water body, enhancing further development of a cuspate foreland. Also, intensive sand transport took place near the right corner of the slender water body because of a large aspect ratio of the water body, which induced the formation of a circular lake.
Figure 16.
Mean sand transport flux in Case 1 [13].
5.2. Segmentation of water body given elliptic distribution of probability (Case 2)
In Case 2, wind blew from the direction of 45° with respect to the principal axis of the slender lake, that is, the probability of occurrence of the wind direction is given by an elliptic distribution [13]. Uda et al. [8] predicted the formation of oriented lakes [15] using the BG model and showed that oriented lakes can develop when the probability of occurrence of the wind direction is given by an elliptic distribution. Here, the segmentation of a rectangular water body was predicted, assuming that the probability of occurrence was given by an elliptic distribution.
Figure 17 shows the predicted results of the lake averaged over 103 steps in Case 2 [13]. Cuspate forelands with an asymmetric form had developed on both shores and inclined rightward (leftward) on lower (upper) shorelines in the beginning. Then, the cuspate forelands had merged to increase their size and moved rightward (leftward) on lower (upper) shorelines. These results are in good agreement with those obtained by Uda et al. [5] concerning the development of sand spits and cuspate forelands owing to the shoreline instability. Because the principal axis of the wind direction is at an angle of 45° relative to the shoreline, and the effect of wind blowing from the land to the lake can be neglected along lower shoreline, the oblique component of waves incident from the left had a higher probability than that of waves incident from the right. As a result, rightward sand transport predominantly caused the formation of a cuspate foreland with an asymmetric shape along the y-axis, and rightward movement of the cuspate foreland took place. The formation of a cuspate foreland with an asymmetric shape corresponds to the formation of a lagoon, as shown in Figure 2. Furthermore, the cuspate foreland markedly developed at the right (left) end on the lower (upper) shoreline because of the long fetch distance and large wave intensity after 2 × 104 steps. With time, the cuspate forelands near the end of the lake were connected to the ends and formed a barrier island, whereas the cuspate foreland in the central part markedly extended to the opposite shore. After 5 × 104 steps, the water body on the left side was segmented to have an elliptic form. Finally, three segmented lakes with an elliptic shape were formed. The formation of the lakes with an elliptic shape with parallel principal axes explains the development process of the elliptic lakes observed in Chukchi Sea shown in Figure 1.
Figure 17.
Topographic changes in Case 2 under elliptic distribution of occurrence of wind direction [13].
5.3. Segmentation of a triangular or crescent-shaped water body (Cases 3 and 4)
Figure 18 shows the results of the calculation of the segmentation of a triangular water body, assuming that the probability of occurrence of wind direction was given by a circular distribution [7]. Although the results are similar to those in [7], numerical simulation was carried out with changing the size of the lake because of the revision in Eq. (2b). Segmentation rapidly occurred in the vicinity of the right end of the triangular water body, and elliptic lakes were formed in the area between y = 3.25 and 3.75 km in the beginning. Near the left end, the segmentation stage was delayed, and cuspate forelands extended from both shores. After 1 × 104 steps, the elliptic lake that formed near y = 3.0 km became rounded and merged into a larger lake, resulting in a decrease in the aspect ratio. Until 4 × 104 steps, five circular lakes were formed. The shape of the water body after 1 × 104 steps well explains the development of the sand spits in Lake Saroma shown in Figure 5.
Figure 18.
Segmentation of a triangular water body with time.
Similarly, Figure 19 shows the results of the segmentation of a crescent-shaped water body with time. Rapid segmentation occurred in the vicinity of the both ends of the crescent water body in the beginning. In the area between y = 3.25 and 4.0 km, cuspate forelands that developed from both shores were alternately distributed on both shores, in contrast to the symmetric cuspate forelands in the central part. This explains the features observed in the water body facing the Chukchi Sea, as shown in Figure 2. After 1 × 104 steps, sand bars with a hound’s-tooth shape were formed in the area between y = 3.75 and 4.25 km. The segmentation continued over time, and the lakes became rounded as a whole. After 105 steps, circular lakes with a radius corresponding to the initial lake width were formed and stabilized.
Figure 19.
Segmentation of a crescent-shaped water body with time.
5.4. Lakeshore changes in circular lake with a rocky or sandy island
Figure 20 shows the lakeshore changes in Case 5 with a rocky island in a circular lake, assuming that the probability of occurrence of wind direction was given by a circular distribution. Under the condition, a wave-shelter zone was primarily formed on the lee of the island against wind waves incident from x-axis. Sand was transported from the outside of the wave-shelter zone to the inside, and a symmetrical cuspate foreland started to form on the lee of the island. After 5 × 104 steps, the cuspate foreland connected to the island. Because sand was mainly transported from the opposite shore with a longer fetch distance to the lee of the island, the lakeshore on the opposite shore was eroded. Thus, when a rocky island is asymmetrically located at a location in a lake, the formation of a cuspate foreland and erosion on the opposite shore take place at the same time.
Figure 20.
Lakeshore changes behind a rocky island in lake (Case 5).
Figure 21 shows the same results in Case 6. In this case, the wave-sheltering effect due to the island was strengthened than that in Case 5 because of the proximity of the island to the lakeshore, the cuspate foreland rapidly developed together with the formation of a large cuspate foreland. After 5 × 104 steps, a headland with a circular head was formed. Because the distance between the island and lakeshore decreased, the wave-sheltering effect increased, resulting in the greater cuspate foreland behind the island and erosion on the opposite shore.
Figure 21.
Lakeshore changes behind a rocky island in lake (Case 6).
The lakeshore changes in Case 7 with a sandy island in a circular lake are shown in Figure 22. When waves were incident to the sandy island, the island deformed by the action of waves incident from x-axis, which has the longest fetch distance, and slender sand bars extended toward the y-axis. In the wave-shelter zone of this sand bars, double tombolo extended at first, which connected to the slender sand bars. With time, all sand comprised of the island were transported to the lakeshore and merged with the lakeshore. After 5 × 104 steps, a large amount of sand was deposited on the lee of the island, whereas the opposite shore was eroded.
Figure 22.
Lakeshore changes around a sandy island in lake (Case 7).
Figure 23 shows the same results in Case 8. The initial circular island significantly deformed owing to the action of wind waves incident from the direction of x-axis, and sand bars extending to the direction of the y-axis were formed. Because of the short distance between the island and lakeshore, double tombolo quickly extended on the lee of the sandy island, while leaving a lagoon in the central part. With time, a barrier island was formed with a lagoon inside double tombolo, and the smaller lake behind the barrier island was rounded by wind waves in the closed water body. A large amount of sand was deposited behind the island.
Figure 23.
Lakeshore changes around a sandy island in lake (Case 8).
The mean sand transport fluxes averaged over 1000 steps between 1.9 × 104 + 1 and 2 × 104 steps in Cases 5 and 7 with the same arrangement of an island are shown in Figure 24. In Case 5 with a rocky island, the intensive sand transport flux occurred on both sides of the island with decreasing the intensity behind the island, whereas in Case 7, strong sand transport flux toward the tips of the sand bar occurred along the shoreline of sand bars. When setting point O at the center of the circular lake, and points a and b at both ends of the straight line through point O, as shown in Figure 24, the direction of sand transport flux is downward at points a and b. Out of waves incident to point a, waves incident from the upper half of the lake causes downward longshore sand transport, and vice versa, when waves are incident from the lower half. Without an island, net sand transport at point A is 0 because of the symmetricity of the closed water body. With an island, however, the area of the water body in the lower half decreases than that in the upper half, resulting in weaker wave action. As a result, the direction of the net sand transport fluxes at points a and b became downward, enhancing sand transport from the upper half to the lower half, resulting in erosion in the upper half.
Figure 24.
Mean sand transport flux averaged over 1000 steps in Cases 5 and 7.
In the case of Lake Balkhash, part of sand comprised of the island was considered to be transported northwestward, forming a long slender sand bar. Such topographic changes can be explained by the mergence of a slender sand bar extended from the island and the sand bar extended in the opposite direction, as shown in the results after 5 × 104 steps in Case 5 and after 2 × 104 steps in Case 7.
6. Conclusions
Specific geomorphological features associated with shoreline instability under a high-wave-angle condition on the lakeshore, such as the development of sand spits, in several elongated water bodies were investigated, and the segmentation of a water body was numerically predicted using the BG model. It was concluded that a rectangular water body segmented into circular (elliptic) lakes when the probability of occurrence of the wind direction was given by a circular (elliptic) distribution. In each case, the wave-sheltering effect of the cuspate forelands played a primary role. Also, the mergence and segmentation of triangular and crescent-shaped slender water bodies were predicted using the BG model. It was further used for predicting the lakeshore changes when a rocky or sandy island exists in a circular lake. The deformation of a sandy island and mergence of the sandy island to the lakeshore were predicted well.
\n',keywords:"closed water body, wind waves, segmentation, lakeshore changes, BG model, cuspate foreland, island",chapterPDFUrl:"https://cdn.intechopen.com/pdfs/58415.pdf",chapterXML:"https://mts.intechopen.com/source/xml/58415.xml",downloadPdfUrl:"/chapter/pdf-download/58415",previewPdfUrl:"/chapter/pdf-preview/58415",totalDownloads:601,totalViews:121,totalCrossrefCites:1,dateSubmitted:"April 4th 2017",dateReviewed:"November 17th 2017",datePrePublished:"December 20th 2017",datePublished:"May 2nd 2018",dateFinished:null,readingETA:"0",abstract:"In a slender water body with a large aspect ratio, the angle of wind waves relative to the direction normal to the shoreline may exceed 45°, resulting in the emergence of cuspate forelands and the segmentation of the water body. The BG model was used to predict the segmentation of a rectangular water body by wind waves when the probability of occurrence of the wind direction is given by a circular or elliptic distribution, and the segmentation of a rectangular water body into a circular or elliptic lake was predicted in each case. The segmentation of a shallow water body with a triangular or crescent shape was also predicted together with the prediction of lakeshore changes when a rocky or sandy island exists in a circular lake.",reviewType:"peer-reviewed",bibtexUrl:"/chapter/bibtex/58415",risUrl:"/chapter/ris/58415",signatures:"Takaaki Uda, Masumi Serizawa and Shiho Miyahara",book:{id:"6184",title:"Applications in Water Systems Management and Modeling",subtitle:null,fullTitle:"Applications in Water Systems Management and Modeling",slug:"applications-in-water-systems-management-and-modeling",publishedDate:"May 2nd 2018",bookSignature:"Daniela Malcangio",coverURL:"https://cdn.intechopen.com/books/images_new/6184.jpg",licenceType:"CC BY 3.0",editedByType:"Edited by",editors:[{id:"205577",title:"Dr.",name:"Daniela",middleName:null,surname:"Malcangio",slug:"daniela-malcangio",fullName:"Daniela Malcangio"}],productType:{id:"1",title:"Edited Volume",chapterContentType:"chapter",authoredCaption:"Edited by"}},authors:[{id:"13491",title:"Dr.",name:"Takaaki",middleName:null,surname:"Uda",fullName:"Takaaki Uda",slug:"takaaki-uda",email:"uda@pwrc.or.jp",position:null,institution:{name:"Tokyo Institute of Technology",institutionURL:null,country:{name:"Japan"}}},{id:"122917",title:"Dr.",name:"Masumi",middleName:null,surname:"Serizawa",fullName:"Masumi Serizawa",slug:"masumi-serizawa",email:"coastseri@nifty.com",position:null,institution:{name:"Tokyo Institute of Technology",institutionURL:null,country:{name:"Japan"}}},{id:"208350",title:"Ms.",name:"Shiho",middleName:null,surname:"Miyahara",fullName:"Shiho Miyahara",slug:"shiho-miyahara",email:"qqqu4vdd@aroma.ocn.ne.jp",position:null,institution:null}],sections:[{id:"sec_1",title:"1. Introduction",level:"1"},{id:"sec_2",title:"2. Examples of cuspate forelands in lake",level:"1"},{id:"sec_2_2",title:"2.1. Lakeshore in Lagoa de Mangueira",level:"2"},{id:"sec_3_2",title:"2.2. Lakeshore in Lake Saroma",level:"2"},{id:"sec_4_2",title:"2.3. Lakeshore in Lake Kitaura",level:"2"},{id:"sec_5_2",title:"2.4. Lake Balkhash",level:"2"},{id:"sec_7",title:"3. Model for predicting lakeshore changes",level:"1"},{id:"sec_8",title:"4. Calculation conditions",level:"1"},{id:"sec_9",title:"5. Results",level:"1"},{id:"sec_9_2",title:"5.1. Segmentation of water body given circular distribution of probability (Case 1)",level:"2"},{id:"sec_10_2",title:"5.2. Segmentation of water body given elliptic distribution of probability (Case 2)",level:"2"},{id:"sec_11_2",title:"5.3. Segmentation of a triangular or crescent-shaped water body (Cases 3 and 4)",level:"2"},{id:"sec_12_2",title:"5.4. Lakeshore changes in circular lake with a rocky or sandy island",level:"2"},{id:"sec_14",title:"6. Conclusions",level:"1"}],chapterReferences:[{id:"B1",body:'Ashton A, Murray AB, Arnault O. Formation of coastline features by large–scale instabilities induced by high-angle waves. Nature. 2001;414:296-300'},{id:"B2",body:'Ashton A, Murray AB High-angle wave instability and emergent shoreline shapes: 1. Modeling of sand waves, flying spits, and capes. Journal of Geophysics Research. 2006;111:F04011. DOI: 10.1029/2005JF000422'},{id:"B3",body:'Zenkovich VP. Processes of Coastal Development. New York: Interscience Publishers; 1967. p. 751'},{id:"B4",body:'Ashton A, Murray AB, Littlewood R, Lewis DA, Hong P. Fetch limited self-organization of elongate water bodies. Geology. 2009;37:187-190'},{id:"B5",body:'Uda T, Serizawa M, Miyahara S. Numerical simulation of three-dimensional segmentation of elongated water body using BG model. Proc. 33rd ICCE, sediment. 65, 2012. pp. 1-11'},{id:"B6",body:'Serizawa M, Uda T, San-nami T, Furuike K. Three-dimensional model for predicting beach changes based on Bagnold’s concept. Proc. 30th ICCE, 2006; pp. 3155-3167'},{id:"B7",body:'Uda T, Serizawa M, Miyahara S, San-nami T. Prediction of segmentation and mergence of shallow water bodies by wind waves using BG model. Proc. Coastal Dynamics. 2013; Paper No. 166, pp. 1729-1740'},{id:"B8",body:'Uda T, Serizawa M, San-nami T, Miyahara S. Prediction of formation of oriented lakes. Proc. 34th ICCE, ASCE. 2014. pp. 1-12'},{id:"B9",body:'Scheffers AM, Kelletat DH. Lakes of the World with Google Earth: Understanding our Environment. Coastal Research Library, Vol. 16. Switzerland: Springer International Publishing; 2016. p. 293'},{id:"B10",body:'Miyahara S, Uda T, Serizawa M, San-nami T. Prediction of effects of artificial alteration on segmentation of a slender water body. Coastal Sediments ‘15. 2015;164:1-14'},{id:"B11",body:'Wilson BW. Numerical prediction of ocean waves in the North Atlantic for December, 1959. Deut. Hydrogr. Zeit, Jahrgang 18, Heft 3. 1965. pp. 114-130'},{id:"B12",body:'Goda Y. Revisiting Wilson’s formulas for simplified wind-wave prediction, Journal of Waterway. Port, Coastal and Ocean Engineering. 2003;129(2):93-95'},{id:"B13",body:'Serizawa M, Uda T, Miyahara S. Segmentation of water body given probability of occurrence of wind direction by circular or elliptic distribution. Proc. 35th Conf. Coastal Eng., sediment. 6. 2016. pp. 1-15'},{id:"B14",body:'San-nami T, Uda T, Gibo M, Ishikawa T, Miyahara S, Serizawa M. Change in carbonate beach triggered by construction of a bridge on Irabu Island and its simulation using BG model. Asian and Pacific Coasts 2013, Proc. 7th International Conf. 2013. pp. 24-31'},{id:"B15",body:'Seppälä M. Wind as a Geomorphic Agent in Cold Climates. New York: Cambridge University Press; 2004. p. 358'}],footnotes:[],contributors:[{corresp:null,contributorFullName:"Takaaki Uda",address:null,affiliation:'
Head, Shore Protection Research, Public Works Research Center, Taito, Japan
Coastal Engineering Laboratory Co., Ltd., Shinjuku, Japan
'}],corrections:null},book:{id:"6184",title:"Applications in Water Systems Management and Modeling",subtitle:null,fullTitle:"Applications in Water Systems Management and Modeling",slug:"applications-in-water-systems-management-and-modeling",publishedDate:"May 2nd 2018",bookSignature:"Daniela Malcangio",coverURL:"https://cdn.intechopen.com/books/images_new/6184.jpg",licenceType:"CC BY 3.0",editedByType:"Edited by",editors:[{id:"205577",title:"Dr.",name:"Daniela",middleName:null,surname:"Malcangio",slug:"daniela-malcangio",fullName:"Daniela Malcangio"}],productType:{id:"1",title:"Edited Volume",chapterContentType:"chapter",authoredCaption:"Edited by"}}},profile:{item:{id:"258432",title:"Dr.",name:"Deyu",middleName:null,surname:"Lin",email:"dashing_lin@126.com",fullName:"Deyu Lin",slug:"deyu-lin",position:null,biography:null,institutionString:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",totalCites:0,totalChapterViews:"0",outsideEditionCount:0,totalAuthoredChapters:"1",totalEditedBooks:"0",personalWebsiteURL:null,twitterURL:null,linkedinURL:null,institution:null},booksEdited:[],chaptersAuthored:[{title:"The Game Theory: Applications in the Wireless Networks",slug:"the-game-theory-applications-in-the-wireless-networks",abstract:"Recent years have witnessed a lot of applications in the computer science, especially in the area of the wireless networks. The applications can be divided into the following two main categories: applications in the network performance and those in the energy efficiency. The game theory is widely used to regulate the behavior of the users; therefore, the cooperation among the nodes can be achieved and the network performance can be improved when the game theory is utilized. On the other hand, the game theory is also adopted to control the media access control protocol or routing protocol; therefore, the energy exhaust owing to the data collision and long route can be reduced and the energy efficiency can be improved greatly. In this chapter, the applications in the network performance and the energy efficiency are reviewed. The state of the art in the applications of the game theory in wireless networks is pointed out. Finally, the future research direction of the game theory in the energy harvesting wireless sensor network is presented.",signatures:"Deyu Lin, Quan Wang and Pengfei Yang",authors:[{id:"258432",title:"Dr.",name:"Deyu",surname:"Lin",fullName:"Deyu Lin",slug:"deyu-lin",email:"dashing_lin@126.com"},{id:"259049",title:"Prof.",name:"Quan",surname:"Wang",fullName:"Quan Wang",slug:"quan-wang",email:"2325343458@qq.com"},{id:"261098",title:"Dr.",name:"Pengfei",surname:"Yang",fullName:"Pengfei Yang",slug:"pengfei-yang",email:"846393016@qq.com"}],book:{title:"Game Theory",slug:"game-theory-applications-in-logistics-and-economy",productType:{id:"1",title:"Edited Volume"}}}],collaborators:[{id:"14847",title:"Prof.",name:"Gershon",surname:"Wolansky",slug:"gershon-wolansky",fullName:"Gershon Wolansky",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"147959",title:"Dr.",name:"Jingtao",surname:"Shi",slug:"jingtao-shi",fullName:"Jingtao Shi",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"237273",title:"Dr.",name:"Torkel",surname:"Bjørnskau",slug:"torkel-bjornskau",fullName:"Torkel Bjørnskau",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"240063",title:"Dr.",name:"Baseem",surname:"Khan",slug:"baseem-khan",fullName:"Baseem Khan",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"248905",title:"Dr.",name:"Jianbo",surname:"Zhang",slug:"jianbo-zhang",fullName:"Jianbo Zhang",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"248908",title:"Prof.",name:"Alain",surname:"Chateauneuf",slug:"alain-chateauneuf",fullName:"Alain Chateauneuf",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"255396",title:"Prof.",name:"Penelope",surname:"Hernandez",slug:"penelope-hernandez",fullName:"Penelope Hernandez",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"255397",title:"MSc.",name:"Adriana",surname:"Alventosa",slug:"adriana-alventosa",fullName:"Adriana Alventosa",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"259049",title:"Prof.",name:"Quan",surname:"Wang",slug:"quan-wang",fullName:"Quan Wang",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"261098",title:"Dr.",name:"Pengfei",surname:"Yang",slug:"pengfei-yang",fullName:"Pengfei Yang",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null}]},generic:{page:{slug:"our-story",title:"Our story",intro:"
The company was founded in Vienna in 2004 by Alex Lazinica and Vedran Kordic, two PhD students researching robotics. While completing our PhDs, we found it difficult to access the research we needed. So, we decided to create a new Open Access publisher. A better one, where researchers like us could find the information they needed easily. The result is IntechOpen, an Open Access publisher that puts the academic needs of the researchers before the business interests of publishers.
",metaTitle:"Our story",metaDescription:"The company was founded in Vienna in 2004 by Alex Lazinica and Vedran Kordic, two PhD students researching robotics. While completing our PhDs, we found it difficult to access the research we needed. So, we decided to create a new Open Access publisher. A better one, where researchers like us could find the information they needed easily. The result is IntechOpen, an Open Access publisher that puts the academic needs of the researchers before the business interests of publishers.",metaKeywords:null,canonicalURL:"/page/our-story",contentRaw:'[{"type":"htmlEditorComponent","content":"
We started by publishing journals and books from the fields of science we were most familiar with - AI, robotics, manufacturing and operations research. Through our growing network of institutions and authors, we soon expanded into related fields like environmental engineering, nanotechnology, computer science, renewable energy and electrical engineering, Today, we are the world’s largest Open Access publisher of scientific research, with over 4,200 books and 54,000 scientific works including peer-reviewed content from more than 116,000 scientists spanning 161 countries. Our authors range from globally-renowned Nobel Prize winners to up-and-coming researchers at the cutting edge of scientific discovery.
\\n\\n
In the same year that IntechOpen was founded, we launched what was at the time the first ever Open Access, peer-reviewed journal in its field: the International Journal of Advanced Robotic Systems (IJARS).
\\n\\n
The IntechOpen timeline
\\n\\n
2004
\\n\\n
\\n\\t
Intech Open is founded in Vienna, Austria, by Alex Lazinica and Vedran Kordic, two PhD students, and their first Open Access journals and books are published.
\\n\\t
Alex and Vedran launch the first Open Access, peer-reviewed robotics journal and IntechOpen’s flagship publication, the International Journal of Advanced Robotic Systems (IJARS).
\\n
\\n\\n
2005
\\n\\n
\\n\\t
IntechOpen publishes its first Open Access book: Cutting Edge Robotics.
\\n
\\n\\n
2006
\\n\\n
\\n\\t
IntechOpen publishes a special issue of IJARS, featuring contributions from NASA scientists regarding the Mars Exploration Rover missions.
\\n
\\n\\n
2008
\\n\\n
\\n\\t
Downloads milestone: 200,000 downloads reached
\\n
\\n\\n
2009
\\n\\n
\\n\\t
Publishing milestone: the first 100 Open Access STM books are published
\\n
\\n\\n
2010
\\n\\n
\\n\\t
Downloads milestone: one million downloads reached
\\n\\t
IntechOpen expands its book publishing into a new field: medicine.
\\n
\\n\\n
2011
\\n\\n
\\n\\t
Publishing milestone: More than five million downloads reached
\\n\\t
IntechOpen publishes 1996 Nobel Prize in Chemistry winner Harold W. Kroto’s “Strategies to Successfully Cross-Link Carbon Nanotubes”. Find it here.
\\n\\t
IntechOpen and TBI collaborate on a project to explore the changing needs of researchers and the evolving ways that they discover, publish and exchange information. The result is the survey “Author Attitudes Towards Open Access Publishing: A Market Research Program”.
\\n\\t
IntechOpen hosts SHOW - Share Open Access Worldwide; a series of lectures, debates, round-tables and events to bring people together in discussion of open source principles, intellectual property, content licensing innovations, remixed and shared culture and free knowledge.
\\n
\\n\\n
2012
\\n\\n
\\n\\t
Publishing milestone: 10 million downloads reached
\\n\\t
IntechOpen holds Interact2012, a free series of workshops held by figureheads of the scientific community including Professor Hiroshi Ishiguro, director of the Intelligent Robotics Laboratory, who took the audience through some of the most impressive human-robot interactions observed in his lab.
\\n
\\n\\n
2013
\\n\\n
\\n\\t
IntechOpen joins the Committee on Publication Ethics (COPE) as part of a commitment to guaranteeing the highest standards of publishing.
\\n
\\n\\n
2014
\\n\\n
\\n\\t
IntechOpen turns 10, with more than 30 million downloads to date.
\\n\\t
IntechOpen appoints its first Regional Representatives - members of the team situated around the world dedicated to increasing the visibility of our authors’ published work within their local scientific communities.
\\n
\\n\\n
2015
\\n\\n
\\n\\t
Downloads milestone: More than 70 million downloads reached, more than doubling since the previous year.
\\n\\t
Publishing milestone: IntechOpen publishes its 2,500th book and 40,000th Open Access chapter, reaching 20,000 citations in Thomson Reuters ISI Web of Science.
\\n\\t
40 IntechOpen authors are included in the top one per cent of the world’s most-cited researchers.
\\n\\t
Thomson Reuters’ ISI Web of Science Book Citation Index begins indexing IntechOpen’s books in its database.
\\n
\\n\\n
2016
\\n\\n
\\n\\t
IntechOpen is identified as a world leader in Simba Information’s Open Access Book Publishing 2016-2020 report and forecast. IntechOpen came in as the world’s largest Open Access book publisher by title count.
\\n
\\n\\n
2017
\\n\\n
\\n\\t
Downloads milestone: IntechOpen reaches more than 100 million downloads
\\n\\t
Publishing milestone: IntechOpen publishes its 3,000th Open Access book, making it the largest Open Access book collection in the world
We started by publishing journals and books from the fields of science we were most familiar with - AI, robotics, manufacturing and operations research. Through our growing network of institutions and authors, we soon expanded into related fields like environmental engineering, nanotechnology, computer science, renewable energy and electrical engineering, Today, we are the world’s largest Open Access publisher of scientific research, with over 4,200 books and 54,000 scientific works including peer-reviewed content from more than 116,000 scientists spanning 161 countries. Our authors range from globally-renowned Nobel Prize winners to up-and-coming researchers at the cutting edge of scientific discovery.
\n\n
In the same year that IntechOpen was founded, we launched what was at the time the first ever Open Access, peer-reviewed journal in its field: the International Journal of Advanced Robotic Systems (IJARS).
\n\n
The IntechOpen timeline
\n\n
2004
\n\n
\n\t
Intech Open is founded in Vienna, Austria, by Alex Lazinica and Vedran Kordic, two PhD students, and their first Open Access journals and books are published.
\n\t
Alex and Vedran launch the first Open Access, peer-reviewed robotics journal and IntechOpen’s flagship publication, the International Journal of Advanced Robotic Systems (IJARS).
\n
\n\n
2005
\n\n
\n\t
IntechOpen publishes its first Open Access book: Cutting Edge Robotics.
\n
\n\n
2006
\n\n
\n\t
IntechOpen publishes a special issue of IJARS, featuring contributions from NASA scientists regarding the Mars Exploration Rover missions.
\n
\n\n
2008
\n\n
\n\t
Downloads milestone: 200,000 downloads reached
\n
\n\n
2009
\n\n
\n\t
Publishing milestone: the first 100 Open Access STM books are published
\n
\n\n
2010
\n\n
\n\t
Downloads milestone: one million downloads reached
\n\t
IntechOpen expands its book publishing into a new field: medicine.
\n
\n\n
2011
\n\n
\n\t
Publishing milestone: More than five million downloads reached
\n\t
IntechOpen publishes 1996 Nobel Prize in Chemistry winner Harold W. Kroto’s “Strategies to Successfully Cross-Link Carbon Nanotubes”. Find it here.
\n\t
IntechOpen and TBI collaborate on a project to explore the changing needs of researchers and the evolving ways that they discover, publish and exchange information. The result is the survey “Author Attitudes Towards Open Access Publishing: A Market Research Program”.
\n\t
IntechOpen hosts SHOW - Share Open Access Worldwide; a series of lectures, debates, round-tables and events to bring people together in discussion of open source principles, intellectual property, content licensing innovations, remixed and shared culture and free knowledge.
\n
\n\n
2012
\n\n
\n\t
Publishing milestone: 10 million downloads reached
\n\t
IntechOpen holds Interact2012, a free series of workshops held by figureheads of the scientific community including Professor Hiroshi Ishiguro, director of the Intelligent Robotics Laboratory, who took the audience through some of the most impressive human-robot interactions observed in his lab.
\n
\n\n
2013
\n\n
\n\t
IntechOpen joins the Committee on Publication Ethics (COPE) as part of a commitment to guaranteeing the highest standards of publishing.
\n
\n\n
2014
\n\n
\n\t
IntechOpen turns 10, with more than 30 million downloads to date.
\n\t
IntechOpen appoints its first Regional Representatives - members of the team situated around the world dedicated to increasing the visibility of our authors’ published work within their local scientific communities.
\n
\n\n
2015
\n\n
\n\t
Downloads milestone: More than 70 million downloads reached, more than doubling since the previous year.
\n\t
Publishing milestone: IntechOpen publishes its 2,500th book and 40,000th Open Access chapter, reaching 20,000 citations in Thomson Reuters ISI Web of Science.
\n\t
40 IntechOpen authors are included in the top one per cent of the world’s most-cited researchers.
\n\t
Thomson Reuters’ ISI Web of Science Book Citation Index begins indexing IntechOpen’s books in its database.
\n
\n\n
2016
\n\n
\n\t
IntechOpen is identified as a world leader in Simba Information’s Open Access Book Publishing 2016-2020 report and forecast. IntechOpen came in as the world’s largest Open Access book publisher by title count.
\n
\n\n
2017
\n\n
\n\t
Downloads milestone: IntechOpen reaches more than 100 million downloads
\n\t
Publishing milestone: IntechOpen publishes its 3,000th Open Access book, making it the largest Open Access book collection in the world
\n
\n"}]},successStories:{items:[]},authorsAndEditors:{filterParams:{sort:"featured,name"},profiles:[{id:"6700",title:"Dr.",name:"Abbass A.",middleName:null,surname:"Hashim",slug:"abbass-a.-hashim",fullName:"Abbass A. Hashim",position:null,profilePictureURL:"https://mts.intechopen.com/storage/users/6700/images/1864_n.jpg",biography:"Currently I am carrying out research in several areas of interest, mainly covering work on chemical and bio-sensors, semiconductor thin film device fabrication and characterisation.\nAt the moment I have very strong interest in radiation environmental pollution and bacteriology treatment. The teams of researchers are working very hard to bring novel results in this field. I am also a member of the team in charge for the supervision of Ph.D. students in the fields of development of silicon based planar waveguide sensor devices, study of inelastic electron tunnelling in planar tunnelling nanostructures for sensing applications and development of organotellurium(IV) compounds for semiconductor applications. I am a specialist in data analysis techniques and nanosurface structure. I have served as the editor for many books, been a member of the editorial board in science journals, have published many papers and hold many patents.",institutionString:null,institution:{name:"Sheffield Hallam University",country:{name:"United Kingdom"}}},{id:"54525",title:"Prof.",name:"Abdul Latif",middleName:null,surname:"Ahmad",slug:"abdul-latif-ahmad",fullName:"Abdul Latif Ahmad",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"20567",title:"Prof.",name:"Ado",middleName:null,surname:"Jorio",slug:"ado-jorio",fullName:"Ado Jorio",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:{name:"Universidade Federal de Minas Gerais",country:{name:"Brazil"}}},{id:"47940",title:"Dr.",name:"Alberto",middleName:null,surname:"Mantovani",slug:"alberto-mantovani",fullName:"Alberto Mantovani",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"12392",title:"Mr.",name:"Alex",middleName:null,surname:"Lazinica",slug:"alex-lazinica",fullName:"Alex Lazinica",position:null,profilePictureURL:"https://mts.intechopen.com/storage/users/12392/images/7282_n.png",biography:"Alex Lazinica is the founder and CEO of IntechOpen. After obtaining a Master's degree in Mechanical Engineering, he continued his PhD studies in Robotics at the Vienna University of Technology. Here he worked as a robotic researcher with the university's Intelligent Manufacturing Systems Group as well as a guest researcher at various European universities, including the Swiss Federal Institute of Technology Lausanne (EPFL). During this time he published more than 20 scientific papers, gave presentations, served as a reviewer for major robotic journals and conferences and most importantly he co-founded and built the International Journal of Advanced Robotic Systems- world's first Open Access journal in the field of robotics. Starting this journal was a pivotal point in his career, since it was a pathway to founding IntechOpen - Open Access publisher focused on addressing academic researchers needs. Alex is a personification of IntechOpen key values being trusted, open and entrepreneurial. Today his focus is on defining the growth and development strategy for the company.",institutionString:null,institution:{name:"TU Wien",country:{name:"Austria"}}},{id:"19816",title:"Prof.",name:"Alexander",middleName:null,surname:"Kokorin",slug:"alexander-kokorin",fullName:"Alexander Kokorin",position:null,profilePictureURL:"https://mts.intechopen.com/storage/users/19816/images/1607_n.jpg",biography:"Alexander I. Kokorin: born: 1947, Moscow; DSc., PhD; Principal Research Fellow (Research Professor) of Department of Kinetics and Catalysis, N. Semenov Institute of Chemical Physics, Russian Academy of Sciences, Moscow.\r\nArea of research interests: physical chemistry of complex-organized molecular and nanosized systems, including polymer-metal complexes; the surface of doped oxide semiconductors. He is an expert in structural, absorptive, catalytic and photocatalytic properties, in structural organization and dynamic features of ionic liquids, in magnetic interactions between paramagnetic centers. The author or co-author of 3 books, over 200 articles and reviews in scientific journals and books. He is an actual member of the International EPR/ESR Society, European Society on Quantum Solar Energy Conversion, Moscow House of Scientists, of the Board of Moscow Physical Society.",institutionString:null,institution:{name:"Semenov Institute of Chemical Physics",country:{name:"Russia"}}},{id:"62389",title:"PhD.",name:"Ali Demir",middleName:null,surname:"Sezer",slug:"ali-demir-sezer",fullName:"Ali Demir Sezer",position:null,profilePictureURL:"https://mts.intechopen.com/storage/users/62389/images/3413_n.jpg",biography:"Dr. Ali Demir Sezer has a Ph.D. from Pharmaceutical Biotechnology at the Faculty of Pharmacy, University of Marmara (Turkey). He is the member of many Pharmaceutical Associations and acts as a reviewer of scientific journals and European projects under different research areas such as: drug delivery systems, nanotechnology and pharmaceutical biotechnology. Dr. Sezer is the author of many scientific publications in peer-reviewed journals and poster communications. Focus of his research activity is drug delivery, physico-chemical characterization and biological evaluation of biopolymers micro and nanoparticles as modified drug delivery system, and colloidal drug carriers (liposomes, nanoparticles etc.).",institutionString:null,institution:{name:"Marmara University",country:{name:"Turkey"}}},{id:"61051",title:"Prof.",name:"Andrea",middleName:null,surname:"Natale",slug:"andrea-natale",fullName:"Andrea Natale",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:null},{id:"100762",title:"Prof.",name:"Andrea",middleName:null,surname:"Natale",slug:"andrea-natale",fullName:"Andrea Natale",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:{name:"St David's Medical Center",country:{name:"United States of America"}}},{id:"107416",title:"Dr.",name:"Andrea",middleName:null,surname:"Natale",slug:"andrea-natale",fullName:"Andrea Natale",position:null,profilePictureURL:"//cdnintech.com/web/frontend/www/assets/author.svg",biography:null,institutionString:null,institution:{name:"Texas Cardiac Arrhythmia",country:{name:"United States of America"}}},{id:"64434",title:"Dr.",name:"Angkoon",middleName:null,surname:"Phinyomark",slug:"angkoon-phinyomark",fullName:"Angkoon Phinyomark",position:null,profilePictureURL:"https://mts.intechopen.com/storage/users/64434/images/2619_n.jpg",biography:"My name is Angkoon Phinyomark. I received a B.Eng. degree in Computer Engineering with First Class Honors in 2008 from Prince of Songkla University, Songkhla, Thailand, where I received a Ph.D. degree in Electrical Engineering. My research interests are primarily in the area of biomedical signal processing and classification notably EMG (electromyography signal), EOG (electrooculography signal), and EEG (electroencephalography signal), image analysis notably breast cancer analysis and optical coherence tomography, and rehabilitation engineering. I became a student member of IEEE in 2008. During October 2011-March 2012, I had worked at School of Computer Science and Electronic Engineering, University of Essex, Colchester, Essex, United Kingdom. In addition, during a B.Eng. I had been a visiting research student at Faculty of Computer Science, University of Murcia, Murcia, Spain for three months.\n\nI have published over 40 papers during 5 years in refereed journals, books, and conference proceedings in the areas of electro-physiological signals processing and classification, notably EMG and EOG signals, fractal analysis, wavelet analysis, texture analysis, feature extraction and machine learning algorithms, and assistive and rehabilitative devices. I have several computer programming language certificates, i.e. Sun Certified Programmer for the Java 2 Platform 1.4 (SCJP), Microsoft Certified Professional Developer, Web Developer (MCPD), Microsoft Certified Technology Specialist, .NET Framework 2.0 Web (MCTS). 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