\\n\\n
Released this past November, the list is based on data collected from the Web of Science and highlights some of the world’s most influential scientific minds by naming the researchers whose publications over the previous decade have included a high number of Highly Cited Papers placing them among the top 1% most-cited.
\\n\\nWe wish to congratulate all of the researchers named and especially our authors on this amazing accomplishment! We are happy and proud to share in their success!
Note: Edited in March 2021
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'IntechOpen is proud to announce that 191 of our authors have made the Clarivate™ Highly Cited Researchers List for 2020, ranking them among the top 1% most-cited.
\n\nThroughout the years, the list has named a total of 261 IntechOpen authors as Highly Cited. Of those researchers, 69 have been featured on the list multiple times.
\n\n\n\nReleased this past November, the list is based on data collected from the Web of Science and highlights some of the world’s most influential scientific minds by naming the researchers whose publications over the previous decade have included a high number of Highly Cited Papers placing them among the top 1% most-cited.
\n\nWe wish to congratulate all of the researchers named and especially our authors on this amazing accomplishment! We are happy and proud to share in their success!
Note: Edited in March 2021
\n'}],latestNews:[{slug:"intechopen-partners-with-ehs-for-digital-advertising-representation-20210416",title:"IntechOpen Partners with EHS for Digital Advertising Representation"},{slug:"intechopen-signs-new-contract-with-cepiec-china-for-distribution-of-open-access-books-20210319",title:"IntechOpen Signs New Contract with CEPIEC, China for Distribution of Open Access Books"},{slug:"150-million-downloads-and-counting-20210316",title:"150 Million Downloads and Counting"},{slug:"intechopen-secures-indefinite-content-preservation-with-clockss-20210309",title:"IntechOpen Secures Indefinite Content Preservation with CLOCKSS"},{slug:"intechopen-expands-to-all-global-amazon-channels-with-full-catalog-of-books-20210308",title:"IntechOpen Expands to All Global Amazon Channels with Full Catalog of Books"},{slug:"stanford-university-identifies-top-2-scientists-over-1-000-are-intechopen-authors-and-editors-20210122",title:"Stanford University Identifies Top 2% Scientists, Over 1,000 are IntechOpen Authors and Editors"},{slug:"intechopen-authors-included-in-the-highly-cited-researchers-list-for-2020-20210121",title:"IntechOpen Authors Included in the Highly Cited Researchers List for 2020"},{slug:"intechopen-maintains-position-as-the-world-s-largest-oa-book-publisher-20201218",title:"IntechOpen Maintains Position as the World’s Largest OA Book Publisher"}]},book:{item:{type:"book",id:"1369",leadTitle:null,fullTitle:"Changing Diversity in Changing Environment",title:"Changing Diversity in Changing Environment",subtitle:null,reviewType:"peer-reviewed",abstract:"As everybody knows, the dynamic interactions between biotic and abiotic factors, as well as the anthropic ones, considerably affect global climate changes and consequently biology, ecology and distribution of life forms of our planet. These important natural events affect all ecosystems, causing important changes on biodiversity. Systematic and phylogenetic studies, biogeographic distribution analysis and evaluations of diversity richness are focal topics of this book written by international experts, some even considering economical effects and future perspectives on the managing and conservation plans.",isbn:null,printIsbn:"978-953-307-796-3",pdfIsbn:"978-953-51-4406-9",doi:"10.5772/1835",price:139,priceEur:155,priceUsd:179,slug:"changing-diversity-in-changing-environment",numberOfPages:404,isOpenForSubmission:!1,isInWos:1,hash:"a9f3c1cbb7119a88079a1c07838455f8",bookSignature:"Oscar Grillo and Gianfranco Venora",publishedDate:"November 14th 2011",coverURL:"https://cdn.intechopen.com/books/images_new/1369.jpg",numberOfDownloads:41287,numberOfWosCitations:115,numberOfCrossrefCitations:22,numberOfDimensionsCitations:93,hasAltmetrics:0,numberOfTotalCitations:230,isAvailableForWebshopOrdering:!0,dateEndFirstStepPublish:"November 23rd 2010",dateEndSecondStepPublish:"December 21st 2010",dateEndThirdStepPublish:"April 27th 2011",dateEndFourthStepPublish:"May 27th 2011",dateEndFifthStepPublish:"July 26th 2011",currentStepOfPublishingProcess:5,indexedIn:"1,2,3,4,5,6,8,9",editedByType:"Edited by",kuFlag:!1,editors:[{id:"51992",title:"PhD.",name:"Oscar",middleName:null,surname:"Grillo",slug:"oscar-grillo",fullName:"Oscar Grillo",profilePictureURL:"https://mts.intechopen.com/storage/users/51992/images/1749_n.jpg",biography:"Dr. Oscar Grillo is a food technologist with an international PhD in applied and environmental botany. Since 2003 he has been working as a researcher at the Stazione Sperimentale di Granicoltura per la Sicilia, a governmental institute of agronomic research, mainly working with computer vision applied to food matrices and plant structures. Currently, he is collaborating with the Sardinian Germplasm Bank of the Biodiversity Conservation Centre of the University of Cagliari on projects devoted to wild plant seed characterization and identification by image analysis. He also works as a supervisor for many MSc and PhD students. He is the author of about 50 research works published in many peer-reviewed journals and about 70 international conference papers. Dr. Grillo is a referee for a few peer-reviewed journals, and many times was invited as a visiting professor by national and international universities and research centres. In 2011 he was the co-editor of five volumes published by InTech, and in 2014 the editor of the last one.",institutionString:null,position:null,outsideEditionCount:0,totalCites:0,totalAuthoredChapters:"1",totalChapterViews:"0",totalEditedBooks:"7",institution:null}],equalEditorOne:null,equalEditorTwo:null,equalEditorThree:null,coeditorOne:{id:"54656",title:"Dr.",name:"Gianfranco",middleName:null,surname:"Venora",slug:"gianfranco-venora",fullName:"Gianfranco Venora",profilePictureURL:"https://mts.intechopen.com/storage/users/54656/images/1750_n.jpg",biography:"Gianfranco Venora is a biologist, born in Caltagirone (Sicily) in 1958, where he lives and works. He took his University degree in 1981, and since 1982 he has been working as researcher at the Stazione Sperimentale di Granicoltura per la Sicilia. His working expertise is mainly about durum wheat and leguminous breeding. At the beginning of 1990, after some years of experience on karyotyping cropped and wild species of agronomical importance, he was fascinated by computer vision applied to food matrices and plant structures, above all seeds, studying wheat and the related leguminous.\nHe was recently nominated as professor to the research doctorate on Applied and Environmental Botany of the University of Cagliari.\nMany peer-reviewed journals published his papers and he was invited as speaker in many international conferences, and as teacher/lecturer by some universities and research centres in Germany, Netherlands, Bulgaria, Spain, Czech Republic and Italy. 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If there are chemical, physical, or biological factors that cause mutations in such genes, these genes are mostly upregulated leading to high cellular proliferation and finally cancer. KRAS is an oncogene. It belongs to the Ras family oncogenes. The proteins expressed by Ras family genes are known to play crucial roles in cell division, cell differentiation, and apoptotic cell death. KRAS can be mutated in several pathological conditions including Cardiofaciocutaneous syndrome, Noonan syndrome, Costello syndrome, Autoimmune Lymphoproliferative Syndrome (ALPS), and epidermal nevus. Moreover, its mutations can be observed in different kinds of cancers, including cancers of the pancreas, lung, and colon. Mutated KRAS has an incidence of ∼50% in colorectal cancers. KRAS gene mutations generally indicate a poor prognosis and are associated with resistance to cancer treatment. On the other hand, certain environmental chemicals like organochlorine insecticides, herbicides, N-nitrosamines; polychlorinated biphenyls, and drugs are suggested to lead to mutations in KRAS oncogene.
\r\n\r\n\tThis book will mainly focus on KRAS oncogene, its mutations, KRAS triggering pathways, MAPK pathway, its association with pathological conditions, cancer and environmental chemicals.
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Does somatosensory stimulation in areas of the face and oral cavity promote salivation and recovery of poor salivary glands? We studied the effects of salivary promotion after hand massage and apparatus of vibrotactile stimulation (89 Hz frequency, 9.8 μm amplitude, and 15 min) in normal humans [1]. Namely, we think that the produce of salivation needs effective changes of an autonomic system for salivation following autonomic activity. Quality of saliva is transmuted by autonomic activity of sympathetic or parasympathetic nerve. In sympathetic activity, viscid saliva functions to allow a food bolus to be easily passed from the mouth into the esophagus. Furthermore, in parasympathetic activity, it is also very important function for the sense of taste and for digestion. In particular, as the poor salivation cannot make the food bolus, dysphasia troubles are induced. On the other hand, poor salivation leads to an increase in dental caries and gingivitis. For ill-fitting dentures of deficits of oral function, massage therapists of the salivation need a rehabilitation method for encouraging salivation and orofacial function [2]. Namely, poor salivations following sickness or advanced aging may be recovered by activation of metabolism of salivary glands. We know that the method of facial traditional massage can induce salivation with increased temperature and blood flow by directly stimulating the salivary glands. However, the descriptions of salivary glands massage from the recent Japanese text will generate salivation by extrusion of accumulated salivary from the acinus glands, and approximately totally 10 pushes form at the anterior to posterior regions of the parotid glands. Furthermore, in the textbook, the submandibular gland is pressed about five times by the thumb to grip the soft parts inside the angle of the mandible, and the sublingual gland is pressed about five times by the thumb from under the chin [3]. The traditional method of saliva massages involved pressing the acinar regions depending on saliva accumulated in that region. However, the principal goal of massages is to maintain one’s metabolism. Thus, we think that the real massage must maintain the metabolism of salivary glands at high levels depending on increasing the temperature of facial skin via haptic stimuli, a paratripsis, through the use of the palms of the hand [4]. The real salivary gland massages must be performed to activate the acinar regions. Functional recovery of salivation is encouraged by promotion of the metabolism of the salivary glands, and a rise in metabolism produces with increasing blood circulation in the salivary glands. This increase in circulation also elevates the temperature around the gland which may activate acinus gland cells. Initially, we examined the effect of facial somatosensory stimuli by using of the apparatus of vibrotactile stimuli [1, 5, 6, 7, 8]. Secondly, we tried to carry out hand massages, again. So, we will report the effects of salivation in facial vibrotactile stimuli and facial hand massages.
\nThe Nihon University School of Dentistry provides ethical approval to conduct this pilot clinical study (approval number: 2009-5). All study participants received verbal explanations regarding measurements of hand massages and a vibrotactile apparatus and signed an informed consent. The study participants were again explained about the protection of privacy and personal information and provided the freedom to continue or withdraw their consent.
\nWe performed facial stranger or personal hand stimuli during 3 and 5 min. After performing the stranger or self-massage procedures for 3 or 5 min, we asked for degree of fatigue. We included 40 healthy subjects (age 26.7 ± 2.4; 25 males, 15 females) and examined well-suited massage time and method depending on first 5 min and then 3 min massage. However, normal subjects were always appealed for feeling of fatigue with an exercise for 5 min. Hand massage for 3 min can be divided into stranger and self-massages: own face has been massaged by other person’ hand or by own hand. Personal massage is not able to treat patients with handicap and cerebral apoplexy. So, we focused at the exercise for 3 minutes and stranger massage (hand massage), as shown in Figure 1A.
\nExperimental method. (A) Stranger hand massages performed at 360° roll per 1 s for 3 min. (B-a and -b) 89 Hz and 9.8 μm amplitude vibrotactile stimulation. (C-a) Thermometers on the facial skin, electrodes of electrocardiogram (ECG), and electrical poles of functional near-infrared spectroscopy (fNIRS) in the frontal cortex and the position of electrodes of ECG. (C-b) Photograph of electrical poles of fNIRS and thermistors. (D) The position of cotton rolls into the intraoral cavity. Cotton rolls under the tongue were recorded salivations of the submandibular and lingual glands and cotton rolls on the buccal mucosa of the upper jaw were recorded salivations of the parotid glands.
After a stranger massage (a light touch and paratripsis massage) of the facial skin, we performed a rotation every second to increase the temperature of the skin and thus boost local blood circulation and improve the metabolism of the parotid glands and around the facial skin (Figure 1B).
\nWe performed the resting and stimulating phases during insertion of cotton rolls for each 3 min between 5 and 7 pm under the circadian rhythm. We explored ECG (electrocardiogram), facial skin temperature, total salivations, OxyHb (oxidation hemoglobin) activity of f-NIRS (functional near-infrared spectroscopy) on the frontal cortex and amylase activity between resting and massage phase of the stranger hand massage. We recorded measurement of resting condition for 3 min after each cotton roll was set into the oral cavity, and then after relax of 1 min interval, new cotton roll was fitted into an oral cavity again and we did measurement of stimulating condition for 3 min. The facial skin temperature, RR intervals of ECG and f-NIRS recorded during experiments, and the observational study were measured in each measuring range. Furthermore, we recorded total salivation and saliva amylase activity after each phase of resting, hand massage, and vibrotactile stimulation.
\nApparatus of 89 Hz frequency and 9.8 μm amplitude vibrotactile stimulation was chosen by data of the previous papers [1, 5, 6, 7, 8], as shown in Figure 1B-a, -b. We tried three vibrotactile stimuli, (89, 114, and 180 Hz, and others all of 9.8 μm amplitude), and the best salivation was 89 Hz frequency in comparison with others, as shown in Figure 2. This apparatus was used by poor salivation patients (especially, Sjogrens’s syndrome and so on) and about 50% of patients showed the effect [1]. Stranger hand massage had a limit time to do massage for physical fatigue, so we tried the 89 Hz frequency vibrotactile apparatus for long time of facial stimulation. Furthermore, we recorded facial skin temperature, total salivation, RR intervals of ECG, and saliva amylase activity, too.
\nTotal salivation in resting salivation and vibrotactile stimuli (89, 114, and 180 Hz frequency).
We explored the facial skin temperature, ECG recording, and fNIRS on the frontal cortex for the comparison with resting for 3 min, stranger massage for 3 min, and vibrotactile apparatus for 15 min.
\nFacial skin temperature was measured by thermistor-pots (BioResarch Co.) located on the facial skin of parotid glands of both sides with adhesive tape, as shown in Figure 1C-a, -b. We recorded the temperature through the experiment and analyzed 3 min from start to finish during resting phase, 3 min from start to finish during stranger hand massage, and 15 min from start to finish during the vibrotactile stimulation.
\nThe electrocardiogram (ECG) recording was induced by the standard limb lead. The heart rate was measured by the RR interval rate (time between R and R) and was analyzed by the variance plot and frequency distribution, as shown in Figure 1C-a. On the other hand, in the distribution of frequency measured by RR interval rate, we decided a mean RR interval value in order to show almost monomodal peaks [9].
\nThe mouths of each subject were fitted with rolls of cotton placed on both sides of the mouth at the following sites on the duct openings of the parotid glands of the buccal mucosa near the second upper molar teeth, and under the tongue to collect saliva from the sublingual and submandibular glands for a measurement of total salivation, as shown in Figure 1D. The total salivations indicate the sum of four cotton rolls (both sides of parotid, and submandibular and sublingual glands), as shown in Figure 1D. We measured the resting salivation for 3 min and after a relaxing interval of a minute, we did stranger hand massages salivation for 3 min again. Furthermore, we measured total salivations of the 15 min vibrotactile stimulation after 5 min resting interval of the massage.
\nThe recording was conducted using a functional near-infrared spectroscopy (fNIRS) OEG16 instrument (SpectraTech, Inc., Shelton, CT, USA) from the frontal cortex. As shown in Figure 1C-a, -b, the fNIRS probe assembly consisted of six LEDs as light sources, each of which emitted two kind of wavelengths, 770 and 840 nm, and six photodiodes as detectors. The sources and detectors were symmetrically arranged in an area of 3.0–14.0 cm, with the nearest source-detector separation of 2.0 cm, and measurement points were at 16 points on a frontal cortex. During scanning, a velcro band held the probe assembly securely to the forehead of subjects and extended from ear to ear horizontally and from hairline to eyebrows vertically. Each of the LEDs was turned on in sequence, and the diffuse NIR light from each source was acquired through the cortical region at the nearest detector. Thus, 16 source-detector pairs (channels) in total were measured (Figure 1C-a, -b). The sampling rate across all 16 channels was 0.76 Hz. In particular, we showed a 16-channel computerized analysis (as shown in the previous papers [5, 6, 7]) and the original waves of four channel recording areas in the central parts. Analysis of amount of OxyHb of fNIRS on the frontal cortex is examined by the program of fNIRS Data Viewer, and we explored channels 4, 7, 10, and 13 of the central part of the frontal cortex. Data recorded by the experiment measured the value of integral of four channels in the center frontal cortex, and we calculated mean value of integral of four waves [5, 6, 10, 11].
\nA salivary amylase (α-amylase) activity was measured by salivary amylase monitor (Nipro Co.) provided for chips of salivary amylase monitor. Measurements of saliva amylase activities were recorded after resting, stranger hand massage, and vibrotactile stimulation phases.
\nWe examined the effect of salivation in resting and stimulating stages between the stranger hand massage and vibrotactile apparatus. We focused on a 3 min stranger massage, because a self-massage could not be performed for treating patients with handicap and stroke, and 5 min massage evoked the tired feeling.
\nIn 5 min hand massages, facial skin temperature increased about 2–3°C in both hand massages (stranger and personal). On the other hand, in 3 min stimuli, facial skin temperature increased about 1.5–2.0°C. The tendency of increased facial skin temperature in 3 and 5 min stimuli was almost same; namely, the ratio of increased temperature was dependent on stimulus time. On the other hand, in performance of stranger hand massages for 5 min, each operator complained with feeling of fatigue, and sometimes showed overflowing of salivation in the cotton rolls of the oral cavity. From this result, we abandoned this experiment of 5 min stimulation depending on using of five subjects. Furthermore, the 5 min massage procedure elicited the sure fatigue. So, we focused to 3 min stranger hand massage.
\nIn loading, facial skin temperature showed about 33°C in the insert of cotton rolls in an oral cavity, as shown in Figure 3. This skin temperature may be stimulated by a foreign substance, because facial skin temperature was decreased up to about 32°C in the resting phase after loading. After a resting phase of 3 min stranger massage stage, facial skin temperature in the stranger massage increased from 32.0 to 34.5°C, as shown in Figure 3; namely, stranger massage showed the increase of facial skin temperature from 32.0 to 34.5 in 3 min stimulation.
\nChanges in temperatures on facial skin before and after 3 min resting phase, 3 min stranger massage, and 15 min vibrotactile stimulation. Black circle is right side and white circle is left side.
On the other hand, the apparatus of 89 Hz frequency and 9.8 μm amplitude vibrotactile stimulation was chosen by data of the previous papers [1, 5, 6, 7, 8], as shown in Figure 1. This vibrotactile stimulation was the best salivation in comparison with others, as shown in Figure 2. In the resting phase, facial skin temperature showed about 32°C. Furthermore, the start of 89 Hz vibrotactile stimulation showed about 33°C and after 15 min, it did 34°C; namely, an increase of 1°C spent due to 15 min vibrotactile stimulation, as shown in Figure 3.
\nFirst, we examined the difference between stranger and self-massages of the RR intervals of ECG. However, there were no differences between the RR intervals of ECG of stranger and self-massages. Especially, the RR intervals in 3 min stranger massage had a tendency to decrease (increase of heart rate), and there was a
RR intervals of ECG (A) and total salivation (B) before and after 3 min hand (stranger and self-massage) massage.
However, hand massages, especially stranger one, will evoke sleepiness by the increased temperature, and metabolism will decrease getting sleepy with the non-increased salivation. Especially, hand massage is needed to countermeasure the effectiveness of fight falling asleep.
\nOn the other hand, total salivation showed about 1.2 ml in resting phase during 3 min, 0.5 ml in stranger massage during 3 min, 1.0 ml in self massage during 3 min, and 3.5 ml in 89 Hz vibrotactile stimulation during 15 min, as shown in Figure 4B. Although 3 min hand massages did not show the effect of autonomic activity, 15 min vibrotactile stimulation did it.
\nThe increase toward plus direction of OxyHb is associated with neuronal activities, but when we become sleepy, it is decreased toward below zero [12, 13]. On the other hand, the zero level of OxyHb of fNIRS showed parasympathetic activity from our data [5, 6, 7]. According to the amount of OxyHb of fNIRS, OxyHb in the stranger massage showed the decrease below zero, as shown in Figure 5. The results may be sleepy with decreased OxyHb during the stranger massage. According to analysis of OxyHb activity of fNIRS, during the resting phase and hand stimulation, subjects showed the nonzero number, and during the second half stimulation of 89 Hz vibrotactile apparatus, they showed the zero level. In particular, the below zero level of OxyHb activity coincided with the inducing of sleepy in the stranger massage. We think that the nonzero number is the decreased metabolism with getting sleepy, and the zero level is the parasympathetic activity (2–15 min in 89 Hz vibrotactile stimulation), as shown in Figure 5 and the previous papers [5, 6, 7, 8]; namely, the stranger massage will produce an early excitation (0–2 min) and a late relaxation (3 min), as shown in Figure 5.
\nChanges in OxyHb of fNIRS of resting and stranger massage for 3 min, and vibrotactile stimulation of 89 Hz frequency and 9.8 μm amplitude for 15 min.
In the previous studies [10, 11, 14], measured values with salivary amylase monitor (Nipro Co.) showed the increased value depending on the sympathetic activity; namely, the value of amylase activity measured by salivary amylase monitor is shown as an increase of value following increased sympathetic activity. The results showed that the minimum value was before hand massage (about 15 KIU/L) and then the maximum value was after stranger massage (about 40 KIU/L) and vibrotactile apparatus (about 42 KIU/L), as shown in Figure 6. These findings show that subjects (patients) may be excited (decreased RR intervals, as shown in Figure 4A) by stranger’s hand touching (Figure 4B). Furthermore, it may be related to an amount of amylase.
\nChanges in amylase activities of loading, resting phase, and hand stranger massage for 3 min, and vibrotactile stimulation of 89 Hz frequency and 9.8 μm amplitude for 15 min.
Firstly, although we tried to perform 5 min massage, there were three bad deficits: in 5 min massage, operators complained about being very tired and they cannot handle patients with handicaps and stroke. Furthermore, we performed by the measurement of salivation with the cotton roll method. When we measured the amount salivation of a cotton roll, subjects of 5 min stimulation with heavy salivation often leaked from a cotton roll [8]. So, we focused to 3 min stranger hand massage, and we measured facial skin temperatures after 3 min resting phase and after 3 min stranger hand stimulation phase. In 3 min stranger hand stimulation, facial skin temperature increased about 2.0°C, as shown in Figure 3. In particular, in comparison with before and after facial skin temperatures between resting and hand massage, although the resting phase increased as little as possible, the hand massage showed a big increase in temperature. On the other hand, a 89 Hz vibrotactile stimulation was spent for about 15 min to increase temperature (about 1.0°C), as shown in Figure 3. The finding showed that the stranger hand massage was especially effective in facial skin temperatures. As shown in Figure 3, a 89 Hz vibrotactile stimulation was spent for 15 min for an increase of 1°C [5, 6, 7, 8]. However, hand massages are adequate with 2–3 min for an increase of 1°C, as shown in Figure 3. Although a 89 Hz vibrotactile stimulation needs long time of 4–7 years as effective recovery, hand massage for 3 min may have more effect with a repetition of day after day, as shown in the previous paper [1]. A 89 Hz vibrotactile stimulation was spent for 15 min time for an increase of 1°C, and this apparatus got effective by using at morning and night. However, as hand massage was necessary for 1–2 min, we may get effect by doing at morning and night; namely, an effective increase in facial skin temperature may be elicited by a good metabolism for recovery [15].
\nThe effect of autonomic activity can directly be studied by changes in RR intervals of ECG and total salivation. The RR interval and salivation are controlled by an autonomic activation, and the increased RR intervals (decrease of heart rate) and a great deal of serous salivation are parasympathetic activity and the decreased ones (increase of heart rate) and a little mucus salivation are sympathetic activity [16, 17]. In the experimental room, the RR interval showed about 700 ms in the resting phase between 0 and 1, and after the resting phase of the latter half, it arrived in about 900 ms, as shown in Figure 4A. This insert of cotton rolls was activated by sympathetic nerve, and the RR intervals were decreased. Furthermore, in the resting phase of the latter half, it became naturalized, and the RR intervals increased, as shown in Figure 4A; namely, it showed the adaptation to the environment in latter resting phase. On the other hand, total salivation was decreased before and after hand massages, as shown in Figure 4B. This decrease may be activated by sympathetic nerve. Three minutes hand massages may be a small amount for the effective autonomic activity and an adequate massage times may produce an effective effort of the autonomic nerve. In the 3 min hand stimulation, they showed the increased rate in average values, and they showed significant differences (T-test,
We have studied an analysis of OxyHb of fNIRS (a functional near-infrared spectroscopy) on the frontal cortex during vibrotactile stimuli, as shown in the previous papers [1, 5, 6, 7, 8]. As a result, we reported that the zero level of the OxyHb of fNIRS showed the parasympathetic activity (Figure 5), and total salivation in the vibrotactile stimulation of the 89 Hz frequency and 9.8 μm amplitude were the most effective.
\nFacial skin temperature increased from 32 to 34°C spend 3 min in the hand massage, and did 15 min in 89 Hz vibrotactile stimulation. Although 3 min stranger massage did not show the effective effect of total salivation, RR intervals increased from 670 to 1000 ms. However, over 3 min massage evoked the fatigue feeling. So, we tried 15 min 89 Hz vibrotactile stimulation. To increase RR intervals, we spent 3 min in the hand massage, but 15 min was spent in the 89 Hz vibrotactile stimulation; namely, an increase of facial skin temperature and RR interval will be effective in the 3 min hand massage.
\nWe measured facial skin temperature and fNIRS on the frontal cortex during 3 min hand stimulation and during 3 and 15 min 89 Hz vibratory stimulation. We reported that the vibrotactile stimuli on the facial skin showed the near zero level of values of OxyHb, DeoxyHb, and TotalHb in fNIRS [1, 5, 6, 7, 8]. The OxyHb and DeoxyHb of brain circulation in the frontal cortex were reported to parallel the neuronal activity [2]. The finding is showed by the increased parasympathetic activity [1, 5, 6, 7, 8]. On the other hand, the decreased OxyHb (under zero level) showed the decreased neuronal activity with the decreased consumption of oxygen and metabolism, and the drowsy and sleepy conditions were shown by the decreased OxyHb during hand massages [13]. According to OxyHb activities of fNIRS on the frontal cortex, effects between stranger massage and resting condition are almost the same under zero level. Hand stimulation for 3 min may not show the increase of total salivation, except for the increase of facial skin temperatures, RR intervals of ECG and saliva amylase. However, RR interval and salivation were effective effort on 15 min 89 Hz vibrotactile stimulation, as shown in Figure 4B and the previous paper [5]. As over 3 min massage produced the fatigue feeling, we thought that repetitious stimuli may change the autonomic system and during hand massage, we tried hard not to get sleepy by talking. However, in the subject, this active feeling was decreased immediately and the subject felt sleepy.
\nA stress is activated by the activation of sympathetic nerve, and an activity of saliva amylase is increased by a self-preservation response of a body; namely, the activity of amylase shows the activity of sympathetic nerve [14]. However, we may relate to amount of amylase because of their mass production after 15 min vibrotactile stimulation, as shown in Figure 6. The results showed the increased activation of saliva amylase related to amount of amylase, too. So, the increased saliva amylase was exhibited by about increase 2.5 times in 3 min hand stimulation and 89 Hz vibrotactile stimulation showed three times, as shown in Figure 6. This finding shows that subjects may be excited by stranger’s hand touching and then decrease of RR intervals (Figure 4B). On the other hand, it may be related to increase of amylase activity and amount of saliva in the 89 Hz vibrotactile stimulation, too.
\nGenerally, a massage is an immediate recovery of reducing stress with warm feeling by a light touch. An explanation in Japanese textbook of “salivation glands massage” was caused by extrusion of accumulated salivary from the acinus glands. However, this method of salivation massage was not encouraged by shakeout of poor glands, we thought. Traditional idea of massage shows immediate recovery of reduced stress with warm feeling. Namely, traditional massage on the facial skin shows immediate reaction, and deactivated salivary glands will be a recovery with an improvement of circulating blood by the increased temperature [18]. The increasing temperature by hand stimuli brings forward metabolism in the facial skin and saliva glands, and deactivated saliva glands as a recovery will be a good tendency. We focused on 3 min hand stranger massage, because 5 min massage was provoked by feeling of fatigue, and self-massage could not treat in handicap and stroke patients. However, we were performed by a hand stranger massage for 3 min, because of operator’s fatigue over 3 min massage. In the effect of automatic nerve system, the hand stranger massage for 3 min increased RR intervals of ECG, did not increase salivation, and increased the amylase activity. However, the hand stranger massage was the best effectiveness of the increased facial skin temperature. On the other hand, hand massages will evoke sleepiness by the increased temperature, and metabolism will decrease getting sleepy with the non-increased salivation. Furthermore, OxyHb of fNIRS on the frontal cortex showed values below zero during hand stimulation. Values below zero in OxyHb of fNIRS show the sleepiness. This reason may suggest that hand massage is effective not only due to increased temperature and metabolism but also non-increased salivation and heart rates. In particular, during hand massage, we must try not to get sleepy by talking. However, the vibrotactile stimulus apparatus for 15 min showed changes in the RR interval of ECG and salivation. On the other hand, repetitious stimuli may change the autonomic system, but the most suitable time of repetitious intervals is necessary for further experiments. As shown in Figure 4A-a, -b, a 89 Hz vibrotactile stimulation is spent for 15 min for an increase of 1°C [5, 6, 7, 8]. However, hand massages are adequate with 2–3 min for an increase of 1°C, as shown in Figure 2A and B. Although the 89 Hz vibrotactile stimulation needs long time of 4–7 years for effective recovery, hand massage for 3 min may have more effect with a repetition of day after day. Namely, an effective increase of facial skin temperature may be elicited by a good metabolism for recovery.
\nIn summary, we showed our idea of salivation by facial somatosensory stimuli, hand massage, and vibrotactile stimulation as shown in Figure 7. Facial somatosensory sense was excited by oral somatosensory inputs with the 89 Hz vibrotactile stimulation or hand massage. Vibrotactile inputs arrived at the hypothalamus via the trigeminal somatosensory nucleus, and then parasympathetic nerves were activated and produced salivation. So, vibrotactile stimulation will be slowly recovered with the increase of facial skin temperature. Although vibrotactile stimulation spends many time for recovery of glands, hand massage might do a short time for recovery. In particular, the hand massage rapidly increased the produced facial skin temperature and reduced the stress. Furthermore, it will recover circulation and metabolism. This massage may be early recovered by a repetitious performing in comparison with a recovery period of the vibrotactile apparatus.
\nOur idea about effects in salivation of facial somatosensory inputs. In summary, we showed our idea of salivation by facial somatosensory stimuli, hand stranger massage, and vibrotactile stimulation. Facial somatosensory sense was excited by oral somatosensory inputs with the 89 Hz vibrotactile stimulation or hand massage. Vibrotactile inputs arrived at the hypothalamus via the trigeminal somatosensory nucleus, and then parasympathetic nerves were activated and produced salivation. So, vibrotactile stimulation will be slowly recovered with the increase of facial skin temperature. Although vibrotactile stimulation spent many time for recovery of glands, hand massage might do a short time for recovery. In particular, the hand stranger massage rapidly increased the produced facial skin temperature and reducing stress. Furthermore, it will recover circulation and metabolism. This massage may be early recovered by a repetitious performing in comparison with a recovery period of the vibrotactile apparatus.
This work was supported by Sato (2018) and Sogoshigaku (2018) research grant of Nihon University School of Dentistry, by Grants-in-Aid for Scientific Research (21592539) and by a grant from the Ministry of Education, Culture, Sports, Science, and Technology to promote multidisciplinary research projects.
\nNone of the authors report any conflict of interest.
Obey dysphasia rehabilitation society.
\nThe Nihon University School of Dentistry provides ethical approval to conduct this pilot clinical study (approval number: 2009-5). All procedures performed in studies involving human participants were in accordance with the ethical standards of the institutional and/or national research committee and with the 1964 Helsinki declaration and its later amendments or comparable ethical standards. This chapter does not contain any studies with animals performed by any of the authors.
\nInformed consent was obtained from all individual participants included in the study.
\nVoltammetry is an electrochemical technique for current-voltage curves, from which electrode reactions at electrode-solution interfaces can be interpreted. Since current-voltage curves, called voltammograms, include sensitive properties of solution compositions and electrode materials, their analysis provides not only chemical structures and reaction mechanisms on a scientific basis but also electrochemical manufacture on an industrial basis. The voltammograms vary largely with measurement time except for steady-state measurements, and so it is important to pay attention to time variables. Voltage is a controlling variable in conventional voltammetry, and the current is a measured one detected as a function of applied voltage at a given time.
\nThe equipment for voltammetry is composed of electrodes, solution, and electric instruments for voltage control. Electrodes and electric instruments are keys of voltammetry. Three kinds of electrodes are desired to be prepared: a working electrode, a counter one, and a reference one. The three will be addressed below.
\nLet us consider a simple experiment in which two electrodes are inserted into a salt-included aqueous solution. When a constant current is applied to the two electrodes, reaction 2H+ + 2e− → H2 may occur at one electrode, and reaction 2OH− → H2O2 + 2e− occurs at the other. The current is the time variation of the electric charge, and hence it is a kind of reaction rate at the electrode. Since the applied current is a sum of the two reaction rates, one being in the positive direction and the other being in the negative, it cannot be attributed to either reaction rate. A technique of attributing the reactions is to use an electrode with such large area that an uninteresting reaction rate may not become a rate-determining step. This electrode is called a counter electrode. The current density at the counter electrode does not specifically represent any reaction rate. In contrast, the current density at the electrode with a small area stands for the interesting reaction rate. This electrode is called a working electrode. It is the potential difference, i.e., voltage, at the working electrode and in the solution that brings about the electrode reaction. However, the potential in the solution cannot be controlled with the working electrode or the counter one. The control can be made by mounting another electrode, called a reference electrode, which keeps the voltage between an electrode and a solution to be constant. However, the constant value cannot be measured because of the difference in phases. A conventionally employed reference electrode is silver-silver chloride (Ag-AgCl) in high concentrated KCl aqueous solution.
\nAn electric instrument of operating the three electrodes is a potentiostat. It has three electric terminals: one being a voltage follower for the reference electrode without current, the second being a current feeder at the counter electrode, and the third being at the working electrode through which the current is converted to a voltage for monitoring. A controlled voltage is applied between the working electrode and the reference one. These functionalities can readily be attained with combinations of operational amplifiers. A drawback of usage of operational amplifiers is a delay of responses, which restricts current responses to the order of milliseconds or 10 kHz frequency.
\nVoltammetry includes various types—linear sweep, cyclic, square wave, stripping, alternating current (AC), pulse, steady-state microelectrode, and hydrodynamic voltammetry—depending on a mode of the potential control. The most frequently used technique is cyclic voltammetry (CV) on a time scale of seconds. In contrast, currently used voltammetry at time as short as milliseconds is AC voltammetry. We describe here the theory and tips for practical use of mainly the two types of voltammetry.
\nThe theory of voltammetry is to obtain expressions for voltammograms on a given time scale or for those at a given voltage. First of all, it is necessary to specify rate-determining steps of voltammograms. There are three types of rate-determining steps under the conventional conditions: diffusion of redox species in solution near an electrode, adsorption on an electrode, and charging processes at the double layer (DL). Electric field-driven mass transport, called electric migration, belongs to rare experimental conditions, and hence it is excluded in this review. When a redox species in solution is consumed or generated at an electrode, it is supplied to or departed from the electrode by diffusion unless solution is stirred. When it is accumulated on the electrode, the change in the accumulated charge by the redox reaction provides the current. Whenever electrode voltage is varied with the time, the charging or discharging of the DL capacitor causes current. Therefore, the three steps are frequently involved in electrochemical measurements.
\nA mass transport problem on voltammetry is briefly described here. The redox species is assumed to be transported by one-directional (
where
The other conditions are concentrations in the bulk (
If the mass transport is controlled only by
where
When the voltage is linearly swept with the time at a given voltage scan rate,
The above Abel’s integral equation can be solved by Laplace transformation. When the time variation is altered to the voltage variation through
where
at
Practical voltage-scan voltammetry is not simply linear sweep but cyclic voltammetry (CV), at which applied voltage is reversed at a given voltage in the opposite direction. The theoretical evaluation of the voltammogram should be at first represented in the integral form with the time variation and then express the time as the voltage. One of the features of the diffusion-controlled cyclic voltammograms is the difference between the anodic peak potential and the cathodic one, Δ
Voltammograms calculated from
AC voltammetry can be performed when the time variation of voltage is given by
A voltammogram (
Voltammogram calculated from
The AC-impedance technique often deals with the real impedance,
Here
When the redox species with reaction R = O + e− is adsorbed on the electrode and has no influence from the redox species in the solution, the sum of the surface concentrations of R and O is a constant,
The time derivative of the redox charge corresponds to the current density,
The voltammogram takes a bell shape (Figure 2), of which peak is at
Since a phase has its own free energy, contact of two phases provides a step-like gap of the free energy, of which gradient brings about infinite magnitude of force. In order to relax the infinity, local free energy varies from one phase to the other as smoothly as possible at the interface. The large variation of the energy is compensated with spontaneously generated space variations of voltage, i.e., the electric field, which works as an electric capacitor. The capacitance at solution-electrode interface causes orientation of dipoles and nonuniform distribution of ionic concentration, of which layer is called an electric double layer (DL).
\nWhen the time variation of the voltage is applied to the DL capacitance,
where
The DL capacitance has exhibited the frequency dispersion expressed by
This is a simple sum of the real part of the current and the imaginary one, indicating that the equivalent circuit should be a parallel combination of a capacitive component and a resistive one, both depending on frequency. Since the ratio, −
If the capacitive charge is independent of the time, the capacitive current should be
Capacitive voltammograms by CV at
The variation of CV computed from Eq. (13) (Figure 3, solid curves) is similar to our conventionally observed capacitive waves.
\nVoltammograms can identify an objective species by comparing a peak potential with a table of redox potentials and furthermore determine its concentration from the peak current. Their results are, however, sometimes inconsistent with data by methods other than electrochemical techniques if one falls in some pitfalls of analytical methods of electrochemistry. For example, a peak potential is influenced by a reference electrode and solution resistance relevant to methods. Peak currents are varied complicatedly with mass transport modes as well as associated chemical reactions. Since the theory on voltammetry covers only some restricted experimental conditions, it can rarely interpret the experimental data successfully. This review is devoted to some voltammetric tips which can lead experimenters to reasonable interpretation.
\nIt is rare to observe a reversible voltammogram in which both oxidation and reduction waves appear in a symmetric form with respect to the potential axis at a similar peak potential, as in Figure 1. Frequently observed voltammograms are irreversible, i.e., either a cathodic or an anodic wave appears; a value of a cathodic peak current is quite different from the anodic one in magnitude; a cathodic peak potential is far from the anodic one. These complications are ascribed to chemical reactions and/or phase transformation after the charge-transfer reaction. A typical example is deposition of metal ions on an electrode. The complications can be interpreted by altering scan rates and reverse potentials.
\nA wave at a backward scan is mostly attributed to electrode reactions generated by experimenters rather than to species latently present in the solution. That is, it is artificial. It is caused either by the reaction of the wave at the forward scan or the reaction of the rising-up current just before the reverse potential. A source of the backward wave can be found by changing the reverse potentials.
\nSome voltammograms have more than two peaks at one-directional scan. The appearance of the two can be interpreted as a two-step sequential charge-transfer reaction. However, multiple waves appear also by combinations of chemical reactions and adsorption. The peak current and the charge for this case are quite different from the predicted ones, as will be described in Section 3.2. Change in scan rates may be helpful for interpreting the multiple waves.
\nIt is possible to predict theoretically a controlling step of voltammograms from their shape (a bell type corresponding to an adsorption wave or a draw-out type corresponding to a diffusion wave). However, the shape strongly depends on chemical complications, adsorption, and surface treatment of the electrodes. When redox species in solution is partially adsorbed on an electrode, the electrode process is far from a prediction because of very high concentration in the adsorbed state. A draw-out-shaped wave can be observed even for the adsorbed control. It is important to estimate which state the reacting species takes on the electrode. Potentials representing of voltammetric features do not express a controlling step in reality although the theory does. One should pay attention to the current. The peak current controlled by diffusion with one-electron transfer is given by
The peak potential difference Δ
It is necessary to pay attention to the validity of analyzing Δ
Voltammograms of a number of redox species have been reported to be diffusion controlled from a relationship between
Plots of
There is a simple method of determining a controlling step either by diffusion or adsorption. Current responding to diffusion-controlled potential at a disk electrode in diameter less than 0.1 mm would become under the steady state after a few seconds [8]. Adsorption-limited current should become zero soon after the potential application. Many redox species, however, show gradual decrease in the current because reaction products generate an adsorbed layer which blocks further electrode reactions.
\nIt is well known that currents vary not only with applied voltage but also with the time. It is not popular, however, to discuss quantitatively time dependence of CV voltammograms. Enhancing
A technique of analyzing the potential shift is to plot
Plots of
Most researchers have quoted the Randles-Sevcik equation,
Let a potential width from a current-rising potential to
An electrochemical response is observed as a sum of the half reactions at the two electrodes. In order to extract the reaction at the working electrode, a conventional technique is to increase the area of the counter electrode so that the reaction at the counter electrode can be ignored. If the counter electrode area is increased by 20 times the area of the working electrode, the observed current represents the reaction of the working electrode with an error of 5%. Let us consider the experiment in which nanoparticles of metal are coated on a working electrode for obtaining capacitive currents or catalyst currents. Then, the actual area of the working electrode can be regarded as the area of the metal particles measured by the molecular level. Then, the area will be several thousand times the geometric area so that the observed current may represent the reaction at the counter electrode. This kind of research has frequently been found in work on supercapacitors. On the other hand, if the electrode reaction is diffusion controlled, the current is determined by the projected area of the diffusion layer. Then the current is not affected by the huge surface area of nanoparticles.
\nIt is important to examine whether or not a reaction is controlled by at a counter electrode. A simple method is to coat nanoparticles also on the counter electrode. Then the current in the solution may become so high that the potential of the working electrode cannot be controlled. It is better to use a two-electrode system. Products at the counter electrode are possible sources of contaminants through redox cycling.
\nThe Ag-AgCl electrode is most frequently used as a reference electrode in aqueous solution because of the stable voltage at interfaces of Ag-AgCl and AgCl-KCl through fast charge-transfer steps, regardless of the magnitude of current density. The “fast step” means the absence of delay of the reaction or being in a quasi-equilibrium. The stability without delay is supported with high concentration of KCl.
\nWhen an Ag-AgCl electrode is inserted to a voltammetric solution, KCl necessarily diffuses into the solution, associated with oxygen from the reference electrode. Thus, the reference electrode is a source of contamination by salt, dichlorosilver and oxygen. It is interesting to examine how much amount a solution is contaminated by a reference electrode [9]. Time variation of ionic conductivity in the pure water was monitored immediately after a commercially available Ag-AgCl electrode was inserted into the solution. Figure 6 shows rapid increase in the conductivity as if a solid of KCl was added to the solution. Oxygen included in the concentrated KCl may contaminate a test solution. Even the Ag-Ag
Time-variation of conductivity of water into which (circles) Ag|AgCl, (triangles) Ag|Ag
When a constant voltage is applied to the ideal capacitance
Chronoamperometric curves when 0.2 V vs. Ag|AgCl was applied to a Pt wire in 0.5 M KCl aqueous solution. Solid curves are fitted ones by exp(-
The slow decay is related with a loss of the performance of pulse voltammetry, in which diffusion-controlled currents can readily be excluded from capacitive currents. The advantage of pulse voltammetry is based on the assumption of the exponential decay of the capacitive current. Since the diffusion current with 1/
High-performance potentiostats are equipped with a circuit for compensation of resistance by a positive feedback. Unfortunately, the circuit is merely useful because voltammograms depend on intensity of compensation resistances of the DL capacitance. It should work well if the DL capacitance is ideal.
\nAC techniques have an advantage of examining time dependence at a given potential, whereas CV has a feature of finding current-voltage curves at a given time. The former shows the dynamic range from 1 Hz to 10 kHz, while the latter does conventionally from 0.01 to 1 Hz. This wide dynamic range of the AC technique is powerful for examining dynamics of electrode reactions. Analytical results by the former are often inconsistent with those by the latter, because of the difference in the time domain. The other scientific advantage of the AC technique is to get two types of independent data set, frequency variations of real components and imaginary ones by the use of a lock-in amplification. The independence allows us to operate mathematically the two data, leading to the data analysis at a level one step higher than CV. An industrial advantage is the rapid measurement, which can be applied to quality control for a number of samples. The analysis of AC impedance necessarily needs equivalent circuits of which components do not have any direction relation with electrochemical variables.
\nData of the electrochemical AC impedance are represented by Nyquist (Cole-Cole) plots, that is, plots of the imaginary component (
(A) Nyquist plots for a RC-series circuit with ideal capacitor (a) and DL capacitor (b). (B) Equivalent circuit with the power-law of
The equivalent circuit with the Randles type is a parallel combination of the ideal DL capacitor
Residual current varies with treatments of electrodes such as polishing of electrode surfaces and voltage applications to an extremely high domain. It can often be suppressed to yield reproducible data when the electrode is replaced by simple platinum wire or carbon rod having the same geometric area. Simple wire electrodes are quite useful especially for measurements of DL capacitance and adsorption. One of the reasons for setting off large residual current is that the insulator of confining the active area is not in close contact with the electrode, so that the solution penetrated into the gap will give rise to capacitive current and floating electrode reactions. Since the coefficient of thermal expansion of the electrode is different from that of the insulator, the residual current tends to get large with the elapse from the fabrication of the electrode. This prediction is based on experience, and there are few quantitative studies on residual currents.
\nUnexpected gap has been a technical problem at dropping mercury electrodes. If solution penetrates the inner wall of the glass capillary containing mercury, observed currents become irreproducible. Water repellency of the capillary tip has been known to improve the irreproducibility in order to reduce the penetration. A similar technique has been used for voltammetry at oil-water interfaces and ionic liquid-water interfaces at present.
\nVoltammograms are said to vary with electrode reaction rates, and the rate constants have been determined from time dependence of voltammograms. The fast reaction of which rate is not rate determining has historically been called “reversible.” In contrast, such a slow reaction that a peak potential varies linearly with log
CV voltammograms (solid curves) at a normally sized electrode and steady-state voltammograms (dashed curves) at a microelectrodes in 12 μm in diameter, calculated theoretically for v = 0.5 V s−1, D = 0.73 × 10−5 cm2 s−1, ks = (a) 0.1, (b) 0.01, (c) 0.001, (d) 0.0001 cm s−1. The potential shift of CV is equivalent to the wave-shift at a microelectrode through the relation, v = 0.4RTD/αFa2 (a: radius).
The authors attempted to find a redox species with the above four behaviors. Some redox species can satisfy one of the four requirements, but do not meet the others. Most reaction rate constants have been determined from the potential shift in a narrow time domain. They are probably caused by follow-up chemical reactions, adsorption, or DL capacitance. For example, CV peak potentials of TCNQ and benzoquinone were shifted at high scan rates, whereas their steady-state voltammograms were independent of diameters of microdisk electrodes even on the nanometer scale [14]. The shift at high scan rates should be due to the frequency dispersion of the DL capacitance, especially the parallel resistance in the DL (Figure 8B). Values of the heterogeneous rate constants and transfer coefficients reported so far have depended not only on the electrochemical techniques but also research groups. Furthermore, they have not been applied or extended to next developing work. These facts inspire us to examine the assumptions and validity of the BV formula.
\nLet us revisit the assumptions of the BV equation when an overvoltage, i.e., the difference of the applied potential from the standard electrode potential, causes the electrode reaction. The rate of the oxidation in the BV equation is assumed to have the activation energy of
Development of scanning microscopes such as STM and AFM has allowed us to obtain the molecularly and atomically regulated surface images, which have been used for interpreting electrochemical data. Then the electrochemical data are expected to be discussed on a molecular scale. However, there is an essential problem of applying photographs of regularly arranged atoms on an electrode to electrochemical data, because the former and the latter include, respectively, microscopically local information and macroscopically averaged one. A STM image showing molecular patterns is information of only a part of electrode, at next parts of which no atomic images are often observed but noisy images are found. Electrochemical data should be composed of information both at a part of the electrode showing the molecular patters and at other parts showing noisy, vague images. Noisy photographs are always discarded for interpreting electrochemical data although the surfaces with noisy images also contribute electrochemical data.
\nAn ideal experiment would be made by taking STM images over all the electrodes that provide electrochemical data and by obtaining an averaged image. However, it is not only impossible to take huge amounts of images, but the averaged image might be also noisy. It may be helpful to describe only a possibility of reflecting the STM-imaged atomic structure on the electrochemical data.
\nVoltammograms by adsorbed redox species, called surface waves, are frequently different from a bell shape (Figure 2). Really observed features are the following: (i) the voltammogram does not suddenly decay after the peak, exhibiting a tail-like diffusional wave; (ii) the peak current and the amount of the electricity are proportional to the power less than the unity of
A loss of the symmetry with respect to the vertical line passing through a peak can be ascribed to the difference in interactions at the oxidized potential domain and at the reduced one. Since redox species takes extremely high concentration in the adsorbed layer, interaction is highly influenced on voltammetric form. When the left-right asymmetry is ascribed to thermodynamic interaction, it has been interpreted not only with Frumkin’s interaction [15] but also Bragg-Williams-like model for the nearest neighboring interactive redox species [16]. On the other hand, most surface waves are asymmetric with respect to the voltage axis even at extremely slow scan rates. This asymmetry cannot be explained in terms of thermodynamics of intermolecular interaction, but should resort to kinetics or a delay of electrode reactions. There seems to be no delay in the electrode reaction of the monomolecular adsorption layer, different from diffusion species. The delay resembles the phenomenon of constant phase element (CPE) or frequency power law of DL capacitance, in that the redox interaction may occur two-dimensionally so that the most stable state can be attained. This behavior belongs to a cooperative phenomenon [17]. A technique of overcoming these complications is to discuss the amount of charge by evaluating the area of the voltammogram. It also includes ambiguity of eliminating background current and assuming the independence of the redox charge from the DL charge.
\nThe simplest theories for voltammetry are limited to the rate-determining steps of diffusion of redox species and reactions of adsorbed species without interaction. Variation of scan rates as well as a reverse potential is helpful for predicting redox species and reaction mechanisms. Furthermore, the following viewpoints are useful for interpreting mechanisms:
comparison of values of experimental peak currents with theoretical ones, instead of discussing Δ
examining the proportionality of
a reference electrode and a counter electrode being a source of contamination in solution;
attention to very slow relaxation of DL capacitive currents;
inclusion of ambiguity in the equivalent circuit with the Randles type.
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