12 principles of green chemistry, green machine building and green tribology.
\\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!
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'IntechOpen is proud to announce that 179 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 252 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!
\n'}],latestNews:[{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"},{slug:"all-intechopen-books-available-on-perlego-20201215",title:"All IntechOpen Books Available on Perlego"},{slug:"oiv-awards-recognizes-intechopen-s-editors-20201127",title:"OIV Awards Recognizes IntechOpen's Editors"},{slug:"intechopen-joins-crossref-s-initiative-for-open-abstracts-i4oa-to-boost-the-discovery-of-research-20201005",title:"IntechOpen joins Crossref's Initiative for Open Abstracts (I4OA) to Boost the Discovery of Research"},{slug:"intechopen-hits-milestone-5-000-open-access-books-published-20200908",title:"IntechOpen hits milestone: 5,000 Open Access books published!"},{slug:"intechopen-books-hosted-on-the-mathworks-book-program-20200819",title:"IntechOpen Books Hosted on the MathWorks Book Program"}]},book:{item:{type:"book",id:"3825",leadTitle:null,fullTitle:"Pharmacology and Nutritional Intervention in the Treatment of Disease",title:"Pharmacology and Nutritional Intervention in the Treatment of Disease",subtitle:null,reviewType:"peer-reviewed",abstract:"Pharmacology and Nutritional Intervention in the Treatment of Disease is a book dealing with an important research field that has worldwide significance. Its aim is to strengthen the research base of this field of investigation as it yields knowledge that has important implications for biomedicine, public health and biotechnology. The book has brought together an interdisciplinary group of contributors and prominent scholars from different parts of the world. The basic purpose of this book was to promote interaction and discussion of problems of mutual interests among people in related fields everywhere. 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He is\nthe director of Education and Research for the Finnish Satellite Center,\nUNESCO; the president of the International Global Society for Nutrition,\nEnvironment, and Health (GSNEH); an editorial board member of the Scientific World Journal; and the committee member of the Finnish Medical\nPhysiological Society",institutionString:null,position:null,outsideEditionCount:0,totalCites:0,totalAuthoredChapters:"8",totalChapterViews:"0",totalEditedBooks:"3",institution:{name:"University of Helsinki",institutionURL:null,country:{name:"Finland"}}}],equalEditorOne:null,equalEditorTwo:null,equalEditorThree:null,coeditorOne:null,coeditorTwo:null,coeditorThree:null,coeditorFour:null,coeditorFive:null,topics:[{id:"1196",title:"Epileptology",slug:"epileptology"}],chapters:[{id:"46445",title:"Epilepsy Treatment and Nutritional Intervention",doi:"10.5772/57484",slug:"epilepsy-treatment-and-nutritional-intervention",totalDownloads:1667,totalCrossrefCites:2,totalDimensionsCites:2,signatures:"Jerzy Majkowski",downloadPdfUrl:"/chapter/pdf-download/46445",previewPdfUrl:"/chapter/pdf-preview/46445",authors:[{id:"169301",title:"Dr.",name:"Jerzy",surname:"Majkowski",slug:"jerzy-majkowski",fullName:"Jerzy Majkowski"}],corrections:null},{id:"46531",title:"Use of Trace Elements and Halotherapy in the Treatment of Human Diseases",doi:"10.5772/58235",slug:"use-of-trace-elements-and-halotherapy-in-the-treatment-of-human-diseases",totalDownloads:2544,totalCrossrefCites:0,totalDimensionsCites:2,signatures:"Vincent S. 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Annous and Joshua B. Gurtler",coverURL:"https://cdn.intechopen.com/books/images_new/2061.jpg",editedByType:"Edited by",editors:[{id:"101172",title:"Dr.",name:"Bassam",surname:"Annous",slug:"bassam-annous",fullName:"Bassam Annous"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}}]},chapter:{item:{type:"chapter",id:"73927",title:"Green Tribology",doi:"10.5772/intechopen.94510",slug:"green-tribology",body:'\nToday, environmental and energy problems have become extremely serious and survival on a global scale. Scientists in all fields pay great attention to solving these problems. By this logic, the boom of recent decades, associated with the formation and development of nanotechnologies, including in relation to tribology and tribotechnics [1, 2].
\nIt is noticeable that tribology has continuously developed into new phases. After opening in 1956, the effect of selective transfer (ST) (“zero-wear” effect) during friction, in tribology for the first time, was a basis to build the whole new paradigm of “friction without wear with minimal energy consumption”, which was denied by all previous practical experience in operating movable coupling and by theoretical constructions of science of the friction and wear solids. At the same time, by the beginning of this century, the concept of “green tribology” was formed, which actually lists all the achievements in the study of the mechanisms of wearlessness (zero-wear) and super-anti-friction, as well as in the development of lubricants for their implementation in practice [3, 4]. In the 21st century and beyond, green tribology is expected to play an increasingly important role and become the key and strategies for solving a series of global problems in energy, environment and resources.
\nIn recent years, there has been a rapid growth in research activities in green tribology field. A fairly large number of articles, world conference reports and academic books in related to this area have been published [2, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15]. However, there are still few publications that expounded the concepts, technological connotations, principles and disciplinary features of green tribology in precise, comprehensive definition and in an all-round way. The first scientific work completely devoted to green tribology, which emphasized the scientific rather than the economic and social aspects was published by M. Nosonovsky and B. Bhushan in 2010 [5].
\nBeing a new field of tribology still in its infancy, an accurate understanding of the fundamentals of green tribology is important from both a scientific and practical point of view. In this regard, the aim of this work is to clarify the fundamental scientific and technological foundations of green tribology based on the analysis and generalization of the research achievements of green tribology.
\nIt has been noted that the concepts in the main development direction of tribology are historically changed as follows (Figure 1).
\nTribology concepts in the new main direction of development [1, 2].
Nowadays, the term “green tribology” has become part of the engineering dictionary. Green tribology is an emerging and actual area in tribological science with more focus on energy saving and environmental protection. Although green tribology is a fairly new concept; however, it already plays an important role in ensuring that all industrial systems can be able to function in an environmentally friendly manner. Green tribology is especially tuned to sustaining an ecological balance and biological effects on contact between surface systems from different materials. Green tribology ensures that any process of friction and wear is as environmentally friendly as possible. Thus, green tribology can be defined as an interdisciplinary field attributed to the broad induction of various concepts such as energy, materials science, green lubrication, and environmental science [8, 9, 10, 11].
\nWe have known the concept of green engineering for a long time. The United States Environmental Protection Agency (USEPA) defines green engineering as “the design, commercialization and application of processes and products that technically and economically reduce sources of pollution and risks that adversely affect human health and the environment”. Speaking of green tribology, one cannot ignore the terms “Green Technology”, “Green Engineering”, “Green Metalworking”, etc., but the first association and historically, the first green science, as applied to science naturally, was “Green Chemistry”. Green engineering and green chemistry are two closely related fields of green tribology that are actively engaged by researchers today [12, 13].
\nSpecifically, green tribology has been identified as an area of engineering that could go beyond its original remit of improving efficiency by minimizing wear and friction in tribological processes to save energy and resources, minimize noise pollution, develop new bio-lubricants. In general, green tribology gives a positive contribution in reducing environmental harm. Inevitably, the term “green tribology” is spoken of in the context of quality of life. According to professor’s Zhang opinion [2]: “Thus, the concepts and objectives of green tribology might be summarized into 3L + 1H, namely, low energy consumption, low discharge (CO2), low environmental cost, and high quality of life. The mission of green tribology is researching and developing tribological technologies to reach the main objectives, thus making the sustained artificial ecosystems of the tribological parts and tribo-systems in the course of a lifecycle”.
\nEmilia Assenova and her colleagues in their work “Green tribology and quality of life” [14] reported: “Nowadays, losses resulting from ignorance of tribology amount to about 6% of the gross national product (GNP) in the United States alone. This figure is around USD 900 milliard annually. As far as China is concerned, they could save above USD 40 milliard per year by the application of green tribology or more than 1.5% of the GNP”. It is clear that the basic goals of green tribology are “friction control, wear reduction and improved lubrication”. Nevertheless, from a socio-economic point of view, it is possible to extend and confirm that the goal and essence of research works in the field of green tribology is to save material resources, improve energy efficiency, decrease emissions, shock absorption, investigate and apply novel natural bio- and eco-lubricants as well as to reduce the harmful effects of technical systems on the environment, and consequently, improve the quality and welfare of society. All advances in green tribology will lead to a high economic efficiency due to reduced waste and increased equipment service life, improved technological and environmental balance, decreased carbon footprint of mechanical systems, as a result, mitigate climate changes, and improve overall sustainability and safety in human life [15].
\nGreen tribology will play an irreplaceable role in saving energy, material resources and environment. Trusted researches reveal that about 23% of energy consumption in the world today is the result of inefficient performance of tribological systems (Figure 2) [16]. In this case, approximately 18–20% of the energy is consumed to solve friction problems, and the remaining 3–5% is used to rebuild, repair and replace parts worn out due to wear and other failures associated with wear. The researchers estimated that by applying advances in green tribology in terms of new surfaces, materials and lubrication technologies, the total global energy loss in tribological systems could be decreased by 18% in the next 8 years and up to 40% in the next 15 years. An additional advantage of environmentally friendly green tribology is a significant reduction in carbon dioxide emissions and economic costs.
\nEnergy consumption, costs and CO2 emissions due to inefficient performance of tribological systems globally [16].
In works [17, 18, 19, 20, 21, 22, 23] the researchers applied green tribology concept using new class of eco-friendly lubricants and materials for manufacturing anti-friction contact surfaces, as a result of which their coefficient of friction is significantly reduced while the wear resistance and longevity are greatly increased.
\nA survey of gross energy consumption in the United States in four main areas: transportation, turbomachinery, power generation and industrial applications showed that savings of about 11% are achieved thanks to recent developments in lubrication and green tribology [24]. Chinese estimated that they could save more than $ 40 billion per year by applying advances in green tribology [25].
\nIf we look at the share of wind energy in the total installed electricity capacity in Europe over the last decade, according to the European Wind Energy Association, it has increased more than quadrupled from 2.2% in 2000 to 10.5% in 2011 thanks to new developments in tribology, in particular as a result of the application of green tribology [26].
\nMany tribological problems can be put under the umbrella of “green tribology” and are mutually beneficial to each other. These problems are primary focus point of researchers and engineers, which include tribological technology that mimics living nature (biomimetic surfaces) and thus is expected to be environment-friendly, the friction and wear control that is important for energy conservation and conversion, environmental aspects of lubrication and surface modification techniques. These problems and aspects will be clarified in more detail in the next section.
\nAs noted above, the interdisciplinary nature of green tribology often integrates aspects of chemical engineering and materials science in order to completely understand both chemistry and mechanics of surface. Since tribology is an interdisciplinary field, the principles of green engineering and green chemistry should also apply to green tribology. However, tribology includes not only chemistry of surfaces, but also other aspects related to the mechanics and physics of surfaces, there is a need to modify these principles.
\nFormulated by Paul Anastas in 1991, the 12 principles of green chemistry into a constant amount (12) upgraded to the 12 principles of green engineering [27, 28], and later, in the 12 principles of green tribology [1] mapped in Table 1.
\nGreen chemistry | \nGreen engineering | \nGreen tribology | \n
---|---|---|
\n
| \n\n
| \n\n
| \n
12 principles of green chemistry, green machine building and green tribology.
These principles of green tribology can be assorted into 5 following groups: Friction, Wear, Lubrication, Material and surface production and treatment, and Tribology in the renewable energy sources.
\n\nFriction (minimization of heat and energy dissipation). Friction is the main source of energy dissipation, most of which is converted to heat. Controlling and minimizing friction, which results in both energy savings and the prevention of damage to the environment owing to heat pollution, is a top priority for green tribology. In addition, the friction in mechanical systems that operate on friction, such as clutches and brakes, also has to be well optimized.
\n\nWear (minimization of wear). This is the second most important task of green tribology. In most technological processes, wear is undesirable, it decreases the lifetime of elements/machine and creates the problems of their recycling/replacements which in turn leads to environmental damage by way of the emission. Wear can also lead to a large waste of material resources. In addition, due to wear, debris in the form of particles is generated, which pollutes the environment and in certain situations can be dangerous to humans.
\nLubrication.Reduction or complete elimination of lubrication and self-lubrication. Lubrication is at the forefront of tribology as it reduces friction and wear. However, lubrication is also hazardous to the environment. It is desirable to reduce the use of lubricants or achieve a self-lubrication regime when no external lubrication is required. Tribological systems in living nature often operate in the self-lubricating mode. For example, the joints form a closed, self-sufficient system. Green tribology prompted researchers to think about self-lubricating materials, which also eliminated the external supply of lubricants.
\n\nNatural lubrication. In green tribology Natural lubricants such as vegetable oils should be used in cases when possible, since they are eco-friendly.
\n\nBiodegradable lubrication. Biodegradable lubricants should also be used when possible to avoid environmental pollution. In particular, water lubrication is an area that has attracted the attention of tribologists in recent years. Lubrication with natural oils is another good option.
\n\nMaterial and surface production and treatment. Sustainable chemistry and green engineering principles. These principles should be observed in the production of new materials, elements, parts, machines for tribological applications, coatings and lubricants.
\n\nBiomimetic approach. Wherever possible, biomimetic surfaces and materials, as well as other biomimetic and biological approaches, should be applied as they tend to be more environmentally friendly. Common engineered surfaces have occasional roughness, which makes friction and wear extremely difficult to overcome. On the other hand, many biological functional surfaces have complex structures with hierarchical roughness that determines their good properties for tribological systems.
\n\nSurface texturing. This technology should be used to provides a way to control many surface properties relevant to making tribo-systems more ecologically friendly.
\n\nEnvironmental implications of coatings. Environmental implications of coatings and other methods of surface modification (texturing, depositions, etc.) should be studied and taken into consideration.
\n\nDesign for degradation. The ultimate degradation and utilization of contact surfaces, coatings, and tribological components should be considered during design.
\n\nReal-time monitoring. Tribological systems should be analyzed and monitored during operation to prevent the formation of hazardous substances.
\nRenewable energy sources (Sustainable energy applications). Sustainable energy applications should be a priority direction for tribological design, as well as engineering design in general.
\nCorrect observation of discussed above principles of green tribology can greatly reduce the environmental impact of tribological process’s products, assist economic development and, consequently, improve respectively the quality of life.
\nGreen tribology includes 3 main areas [1, 2, 5, 14], these are (1) Biomimetics (imitating living nature in order to solve complex human problems) and self-lubricating materials/surfaces; (2) Biodegradable and environmentally friendly lubrication and materials; and (3) Renewable and/or sustainable sources of energy. These 3 focus areas of green tribology aim to ensure a limited impact of tribological processes on the environment and human health. Below is a brief description and discussion about the features, contents, aspects of these areas and their relevance to green tribology.
\n\nBiomimetic and self-lubricating materials/surfaces\n. This is an important area of green tribology, the main task of which is the development and application of tribological technologies that mimic living nature (biomimetic surfaces). Many biological materials have amazing properties (superhydrophobicity, self-cleaning, self-healing, high adhesion, reversible adhesion, high mechanical strength, antireflection, etc.) that can hardly be achieved by conventional engineering methods. These properties of biological and biomimetic materials are reached due to their composite structure and hierarchical multiscale organization. It is noted that hierarchical organization and the ability of biological systems to grow and adapt also ensure a natural mechanism for the repair or healing of insignificant damage in the material. Biomimetic materials are also usually environmentally friendly in a natural way, since they are a natural part of the ecosystem. For this reason, the biomimetic approach in green tribology is especially promising.
\nIn the field of biomimetic surfaces, a number of typical ideas have been proposed: (1) The lotus effect based non-adhesive surfaces; (2) The Gecko effect based materials with the ability of specially structured hierarchical surfaces to exhibit controlled adhesion; (3) Fish-scale effect based micro-structured surfaces for underwater applications, including easy flow due to boundary slip, the suppression of turbulence and anti-biofouling; (4) Oleophobic surfaces capable of repelling organic liquids; (5) Microtextured surfaces for de-icing and anti-icing; (6) Various biomimetic microtextured surfaces to control friction, wear and lubrication; (7) Self-lubricating surfaces, using various principles, including the ability for friction-induced self-organization; (8) Self-repairing surfaces and materials, which are able to heal minor damage (cracks, voids); (9) The “sand fish” lizard effect, able to dive and “swim” in loose sand due to special electromechanical properties of its scale; (10) Nanocomposite materials tailored in such way that they can produce required surface properties, such as self-cleaning, self-lubrication, and self-healing.\n
\n\nFigure 3 shows typical biological and biomimetic surfaces with hair or pillar like surface structures for various functions (Figure 3) [29]. Recently, the mechanisms of sand erosion resistance of the desert scorpion were studied to improve the erosion resistance of components in tribo-systems [30]. It was found that the biological surfaces used for sand erosion resistance of the desert scorpion were built by the special micro-textures such as bumps and grooves.
\nTypical biological and biomimetic surfaces with hair or pillar like surface structures for various functions. (a) The nano to micro hierarchical hair-like surface structure of geckos’ feet for strong adhesion; (b) The nano to micro hierarchical structure of plant leaves for superhydrophobic dewetting properties. (c) The microfabricated polyimide biomimetic hairs bunching together under the van der Waals interaction [29].
In works [31, 32, 33], the authors presented overview and studies of various biomimetic microtextured surfaces to control friction, wear and lubrication. Generally, biomimetic techniques have provided the different surface structures with strong adhesion, high hydrophobic properties, high coefficient of friction, self-lubrication, etc., which can be prospectively applied in green tribology field.
\n\nBiodegradable and environmentally friendly lubrication and materials.\n Advanced biomimetics is biomimicry used to identify best practices from nature on key tribological issues, such as finding improved lubrication solutions [1, 14, 34]. Natural lubrication is very effective at providing low coefficients of friction even at low speeds, and relies entirely on water as the base component, the effectiveness of which is ensured by the presence of many dissolved biomolecules.
\nImitating such constructs of molecules, understanding their tribological performance is helpful. An example is the process of imitating natural lubricants, e.g. glycoproteins in synovial fluid [32]. By imitating this mechanism in the laboratory, molecules were synthesized that spontaneously produce polymer brushes on the surface. Brushes are formed on surfaces in an aqueous medium when end-grafted, water-soluble polymers are located at distance about one radius of gyration (Rg) from each other (Figure 4) [34] and stretch to maximize their interaction with water while reducing their interaction with each other.
\nThe formation of polymer brushes on surfaces [34].
The use of lubricants in machine components poses a serious threat to the environment, since they released into the environment not only contain harmful toxic waste but also contain the wear debris from machine parts. Development of environmentally acceptable lubricant products is one of priority direction in green tribology. Vegetable oils and animal fats have been used as lubricants for a very long time throughout human history. However, following the industrial revolution and the advent of lubricants made from mineral oils, bio-based lubricants have again come to be seen as an environmentally alternative for lubricant production and have only become effective in recent decades.
\nResearchers confirmed that properly formulated bio-lubricants are comparable with mineral based lubricants, so they could be used as an adequate substitution in appropriate cases. Vegetable-oil-based or animal-fat-based lubricants are potentially biodegradable that can be used for engines, hydraulic and metal-cutting applications. Vegetable oils i.e. corn, soybean and coconut oil, can have excellent lubricity, far superior than that of mineral oil [12, 14]. In general, the advantages of using bio-lubricants are non-toxic, biodegradable, renewable resources, good lubricity and high viscosity indices (Table 2) [35], while disadvantages are: oxidative instability, poor low temperature properties, and hydrolytic instability. Applying chemical modification or additives can address these problems of bio-lubricants.
\nOil type | \nEngine oil | \nCoconut oil | \nPalm oil | \n
---|---|---|---|
CO2 (%) | \n4.5 | \n2.9 | \n3.4 | \n
CO (%) | \n0.92 | \n0.67 | \n0.73 | \n
The percentage content of CO and CO2 in exhaust gas lubricated with regular mineral and vegetable oils [35].
In the area of eco-friendly and biodegradable lubrication and materials we should also notice other following interesting ideas:
\n\nHyrdo-lubrication. These are homogeneous lubricants containing water as a functional component. Tribological study and case analyses of the elastomeric bearings lubricated with seawater for marine propeller shaft systems were conducted [36].
\n\nIonic liquids for green molecular lubrication. Ionic liquids (ILs) have been explored as lubricants for various device applications due to their excellent electrical conductivity as well as good thermal conductivity, where the latter allows frictional heating dissipation [37].
\n\nPowder lubrication. Generally, these tend to be much more eco-friendly than the traditional liquid lubricants. Recent researches show that when using some nanoscale additives, such as boric acid and MoS2 nanopowders to natural oils, their lubricity characteristics are significantly improved [38].
\n\nNew eco-friendly coating materials for tribological applications. Recently, special attention has been paid to the development of “green” coatings in tribo-systems, which have improved tribological properties (low friction coefficient, high wear resistance), and therefore, not releasing a lot of worn-out waste into the environment, they are environmentally friendly [1, 2, 6].
\n\nTribology in the Renewable Energy Sources (RES).\n Controlling and minimizing of friction and wear in tribology is important for energy and resources conservation. Sustainable energy applications have become priority of the tribological design, as well as an important area of green tribology. In contrast to the biomimetic approach and environmentally friendly lubrication, RES is not about manufacturing or operation, but about the application of the tribological system in production of renewable eco-friendly energies such as wind energy, marine energy, solar energy, geothermal energy, and so on.
\nIn work [39] Wood et al. carried out the tribological studies on renewable sources of energy, namely three green energy systems: wind, tidal and wave machines. The authors also highlighted the role of design and durability for such large scale engineering systems from sustainability point of view. These systems are sensitive to operation and maintenance costs and thus depend on functioning tribological parts and lubrication. It was noted that weight reduction to reduce tribological and gravity loads would be beneficial for machines designs. Attention should also be paid to the knowing of dynamic loads to predict fatigue life and tribological loads on wind, tidal and wave machines. Structures and properties of tribological components must be considered for the inherent lack of stiffness of the turbines and wave devices.
\nWind turbines have fairly many specific problems related to their tribology, which involve water contamination, electric arcing on generator bearings, wear of the main shaft and gearbox bearings and gears, the erosion of blades due to solid particles, cavitation, rain, hail stones, etc. The most commonly observed and discussed tribological problems in wind turbines are in the transmission system, in the gearbox. They are mainly the result of insufficient lubrication and/or lack of regular maintenance under extreme operating conditions. The solution to this problem is the use of lubricants and/or materials with improved tribological characteristics [40]. REWITEC nano-coatings is a metal treatment that can be applied to gearboxes and bearings during regular operation for restoration of its efficiency and economy. When examining certain micro-pitting areas on the metal surfaces of a wind turbine gear before applying REWITEC and after 6 months of treatment, it was found that the surface damage was filled and the asperities were smoothed out, and thus the surfaces became smoother with higher surface contact area (Figure 5) [2].
\n3D-images of the metal surface before and after treatment with REWITEC 6 months [2].
Tidal power turbines are another important way of producing renewable energy. Besides tidal, the ocean water flow and wave energy and river flow energy (without dams) can be used with the application of special turbines, which provides the same direction of rotation independent of the direction of the current flow. Production processes of tidal, water flow and wave energy involve certain specific tribological problems such as lubrication of machine components (by seawater, oils, and greases), their erosion, corrosion, and biofouling, as well as the interaction between these modes of damage [1, 39].
\nGeothermal energy plants are widely used now, however, their application is limited to the geographical areas at the edges of tectonic plates. There are several specific tribological issues related to the geothermal energy sources which are discussed in the literature [1, 5, 15, 39].
\nGreen tribology as a new area of tribology has a number of challenges. One obvious problem is integration, synergy of its above mentioned focus areas so that they can benefit from each other. Obviously, a lot of researches is needed to integrate the fields of green tribology. Some ideas can be borrowed from the related fields of green chemistry and green engineering, for example, the development of quantitative parameters for assessing the impact of tribological technologies on the environment. It is also important to develop quantitative measures and metrics that would allow us to compare which tribological material, technology, or application is “greener,” i.e., produces lower carbon footprint, less waste from worn-out materials, and less chemical and heat pollution to the environment.
\nGreen tribology should be integrated into world science and contribute to solving global problems such as resource depletion, environmental pollution and climate change. The application of principles of green tribology by itself, of course, will not solve world problems, and only major scientific achievements can become the key to their solution.
\nIn the face of a large number of tribological problems requiring an early solution, which related to the environmental pollution, crisis of energy and resources on global scale, green tribology should be extended in the following directions [2].
Large-scale deployment of existing knowledge, methods, and technologies of green tribology;
Research and development of novel green tribological technologies;
Research and development of tribo-techniques to support diversification and hybridization of renewable and clean energy;
Making the traditional tribo-materials and lubricating materials “green” in the course of a lifecycle, namely, realizing cleaner production or eco-design of the these materials;
Building up the theory and methodology of green tribology.
Consequently, tribologists should devote all their efforts to the investigation, application and development of green tribology, thereby making a valuable contribution to the existence and development of humanity.
\nIt seems expedient, at least briefly, to consider how the achievements that were obtained in the study of self-organizing tribo-systems, and in particular, the “zero-wear” (effect of wearlessness/effect of selective transfer—ST), play a role in the circle of tasks which green tribology is designed to solve.
\nThe effect of ST in friction was registered as opening in 1966, with a priority in 1956. The authors of this discovery – D.N. Garkunov and I.V. Kragelsky – stated that the essence of the observed phenomenon as follows: “…that in the friction of couple copper alloys-steel under boundary lubrication, eliminating the oxidation of copper, there is a phenomenon of ST of a solid solution of copper from copper-alloy to steel and its transfer backwards from steel to copper alloy, with a reduction of the friction coefficient as liquid lubrication and leads to a significant reduction in wear of the friction pair…” [4].
\nIn the closing years of the XX century the “zero-wear” effect is defined as one of the examples of self-organization in frictional interaction in tribological systems [41, 42], and since then, a synergistic approach at his description has become essential.
\nClassical tribo-system for realizing of ST is a system of “copper alloy (bronze or brass) – aqueous or alcoholic solution of glycerol – steel”. The evolution of the tribological properties of this system visually demonstrated the self-organization in friction in ST mode, which is expressed in the ultra-low frequency vibrations of the friction coefficient and of the size of the rubbing bodies (Figure 6 [42]).
\nThe evolution of the tribological properties (1 – friction moment, 2 – the linear wear) in tribo-system brass-glycerol-steel. A (a, b) – running-in; c, d – transition mode; and e – the ST mode [42].
Self-organization in the ST mode during friction is the consequence of the complex tribo-chemical reactions and physico-chemical processes occurred in the area of frictional contact, which lead to the manifestation of unique tribological characteristics: super-antifrictional (friction coefficient ~ 10−3) and without wear (intensity wear ~10−15). This condition of tribo-system was provided by a protective nanocrystalline servovite film made of soft metal with unusual combination of mechanical properties [43]. According to the results of nanoindentation, such a film has “super-hardness” at compression and “super-fluidity” at shear [44].
\nWithin the framework of the I.V. Kragelsky’s molecular-mechanical theory, the providing extremely low friction coefficients and practical absence of wear during friction of solids is possible either at spontaneous generation of wear auto-compensation systems or in the case of friction of perfectly smooth two-dimensional crystals, in which show up only molecular component of the friction force that occurs, such as, during friction of graphene [45].
\nIn the engineering practice, the auto-compensation systems of wear during friction in the ST regime, usually are formed by selecting (a) the materials of tribo-coupling, (b) a composition of lubricants, and (c) a construction of the friction units. As a result of successful material science and engineering solutions, tribosystems are capable of self-organization, in which the process of frictional interaction moved to the nanocrystalline quasi-liquid [3], and thus provides the friction coefficient, which is characterized for hydrodynamic friction, forming nanoclusters with almost perfect crystals, that leads to increases in load capacity and wear resistance of the friction surfaces.
\nIn practice, “zero-wear” functioning of friction is achieved most often by application of metal-plating lubricants in the real friction units: oils, plastic lubricant, self-lubricating materials and coatings [3].
\nThe mechanism of “zero-wear” effect during friction does not follow from the existing theoretical conclusions about the nature of the frictional interaction. Therefore, none of the attempts to propose developed in detail and experimentally substantiated scientific approach to explaining the “zero-wear” effect is currently generally recognized, although works aimed at clarifying the causes of friction without wear have been underway for more than half a century, during which reliable experimental facts have been accumulated and consistent approaches have been proposed that allowed to qualitatively explain the evolution of the tribo-technical characteristics of friction pairs during realization of the ST.
\nCurrently, it has been reliably established that the composition, thickness and properties of servovite film during frictional interaction continuously change so that the extrapolated to the infinity friction surface is a pure copper (Figure 7), whose stability during friction is provided by the absorption of surfactants from the lubricating medium [42, 46].
\nAFM (3D-visualization) of the surface of the servovite transfer film (brass on steel in glycerol) [42].
Detailed studies on tribochemical reactions, as well as the evolution of the chemical composition of the servovite film on friction surfaces in the “zero-wear” regime, made it possible to characterize in detail the products arising during friction and to establish their role in the mechanisms of formation of boundary layers during self-organization of not only the classical tribosystem “copper-glycerin-steel”, but also a number of more effective tribosystems using other lubricants, such as aqueous solutions of polyhydric alcohols, solutions of sucrose, glucose, galactose and other carbohydrates [3].
\nString of sequential and parallel chemical reactions: tribo-oxidation, tribo-coordination, tribo-restoration, tribo-reducing decay of coordination compounds, tribo-polymerization, tribo-clusterization and others, etc., accompanying, and/or generating vibrational tribo-chemical reaction, vibrational electrical and electrochemical effects, vibration of the size of rubbing bodies and tribological characteristics of friction pairs - that’s the one, is far from complete.
\nIn the most general case, the evolution of the open tribo-system “copper alloy-glycerin-steel”, classical for the realization of the “zero-wear” effect, from the thermodynamically equilibrium state of rest under constant external initial conditions (P, V, T) to the friction regime without wear always starts with high (more than 0.1) values of the friction coefficient and large running-in wear, which leads to an increase in the energy intensity of the frictional contact zone and triggers complex physicochemical transformations in the lubricating medium and on the contacting surfaces of copper alloy and steel. At the same time, in the initial period of time, the friction of the copper alloy against steel in glycerin does not differ in nature from the boundary friction, which manifests itself both in the tribo-technical, electrical and electrochemical contact characteristics. The products of wear accumulating at this time in glycerin have a very wide particle size distribution from 10−7 to 10−3 m and are almost exclusively particles softer from contact bodies of copper alloy. Wear, repeatedly increasing surfaces of copper alloy in the tribo-system, leads to the predominant role of topochemical and tribo-chemical effects, both in the lubricant composition and on the friction surfaces, which reflect in the tribo- and topochemical oxidation of glycerin with the accumulation of a wide range of oxygen-containing surfactants (aldehydes, ketones, carboxylic acids, ethers and esters, as well as oligomeric and polymeric products of their further transformations). Parallel to this, the formation of complex compounds (tribo-coordination) occurs both on the surface of wear particles and on the friction surfaces, and the soluble coordination metal compounds accumulate in the solution [3, 47, 48, 49].
\nLeading of tribo-chemical mechanisms on electrochemical reasons on the friction surface and on the surface of wear of particles is oxidation of copper Cu\n0\n- 2e = Cu\n+2 (in the case of bronze) or zinc Zn\n0\n-2e = Zn\n+2 (in the case of brass) in result of its selective dissolution. Other metals that are part of the friction alloys such as Fe, Sn, Pb, etc., are also subjected to tribo-oxidation with the formation of metal-containing products, so that in the lubricating medium and on the frictional surface simultaneously there is a wide gamma of products, in which the explicitly pronounced tendency in the initial period is the accumulation of oxidized forms of different metals and oxidation products of the lubricant. An important event at this stage of evolution is the accumulation in the lubricating medium and reducing the size of the metallic wear particles with a simultaneous change in their composition due to above reasons. This leads ultimately to the accumulation of metal-containing products upto critical concentrations and thus, to the change of lubricant composition in becoming a metal-plating lubricant. There is a radical change of physico-chemical, electrochemical and tribological situation on the friction surfaces and in the zone of frictional contact. Tribo-system in the course of long enough evolution (in the laboratory it is about 103 m of sliding distance) reaches the bifurcation point with transition either to “zero-wear” friction regime or to the regime of the catastrophic wear.
\nIn the transition and functioning of the tribo-system under ST, both contacting surfaces in friction as copper alloy and steel have the same composition and structure. This is another paradox of ST and an unusual combination of materials of the rubbing surfaces. It has been observed that during friction of the same materials (usually in the friction units dissimilar metals and alloys are combined) record-breaking parameters of frictional interaction can be achieved, wherein the self-organization of frictional systems was achieved by the special structure of surface layers.
\nIn the transition from boundary friction to “zero-wear” friction, due to the non-equilibrium character of the processes occurring in the tribo-system (since the system is far enough from the position of thermodynamic equilibrium), and their description by systems of nonlinear differential equations, oscillatory mechanisms begin to appear, which associated with both tribo-chemical transformations in the contact zone, for example, with fluctuations in the concentration of copper-containing products in the lubricant, and with the electrical, electrochemical and tribological characteristics of the contact (Figure 8) [50]. Observing this type of oscillations, which always accompany friction in the “zero-wear” regime, prove the manifestation of the self-organization in friction, as well as the transition and functioning of the tribological system in one of the stationary states.
\nFluctuations in the transient regime of “boundary friction – ST” in the friction pair “AISI 1045 Steel–AISI 1045 Steel” in the lubricant of copper nanocluster in glycerol. 1 – load; 2 – friction coefficient; 3 – electrical resistance of contact [50].
The transient regime from boundary to “zero-wear” friction lasts significantly less than the boundary friction regime, but at this time there are main events that lead to the unique tribological characteristics of tribo-system. It is in this transition that the ordering process occurs, which associated with the formation of a servovite film on the friction surface. The servovite film is formed under nonequilibrium, non-isothermal and topographically unequal conditions, which leads to inevitable differences in its composition and properties in different places of frictional contact. Nevertheless, formation of the film is always due to mutually complementary processes of tribo- and electrochemical reduction of coordination compounds of soft metals on the friction surface, clustering their reduced forms, and optimization depending on the friction regimes (P, V, T), sizes (in the nanoscale) and the shape (triaxial ellipsoid) of the clusters in two ways “top-down” and “bottom-up” followed by the direct deposition of metal nanoclusters on the contact surfaces due to tribo-electrochemical effects. The formation of servovite film begins on the individual most active sections of the steel surface, which leads to reducing the friction coefficient and a decrease in the energy density the friction unit. Finally, it is accompanied by a decrease in wear and a transfer of the film formation process to less activated areas on the frictional contact surfaces.
\nAny system thermodynamically approaches to one of many possible stationary states, the choice of which is caused solely by the initial conditions. It should be noted that the trajectory of the tribo-system during evolution into the “zero-wear” regime is always strictly individual and can never be reproduced in detail. If the tribo-system self-organizes, which in the thermodynamic description is characterized by an increase in entropy and ordering, then its tribological and physicochemical characteristics in a stationary state become almost unchanged (Figure 9) [50].
\nStationary regime in the realization of ST in friction pair “AISI 1045 Steel–AISI 1045 Steel” with lubricant of copper nanocluster in glycerol. 1 – load, 2 – friction coefficient, 3 – electrical resistance of contact [50].
This is due to the fact that a servovite film, formed from individual atoms and their small clusters, has a nanocrystalline structure and, on the one hand, is super-strong in compression, since its nanoparticles are fragments of almost ideal crystals, and on the other hand, the film is quasi-liquid and superplastic under tension and shear due to much weaker interactions between nanoparticles than between atoms in the metal crystal lattice [43].
\nIn this regime, the system can function until continuously accumulating external disturbances or changing external conditions transfer it to a new stationary state, which may be characterized by other and not necessarily higher tribo-technical characteristics, which makes the practical implementation of “zero-wear” in real machines and mechanisms very complex and not always justified event.
\nAt the same time, even with a partial realization of “zero-wear” friction, the effects can be impressive, since when functioning under self-organization conditions and with a slight change in external conditions, the transition to a nearby stationary state is accompanied, as a rule, by a slight change in the tribo-technical properties of the system.
\nThus, the application of “zero-wear” effect in engineering practice opens a real opportunity for the design of friction units with significantly increased durability and ultra-high efficiency in terms of friction losses in moving machine interfaces. The “zero-wear” effect in the friction fully fits into the presentation and concepts of green tribology and should be considered as the real embodiment in the theory and practice of modern engineering.
\nGreen tribology is a novel area of science and technology. It is related to other areas of tribology as well as other “green” disciplines, namely, green engineering and green chemistry. In this chapter the main scientific and technological aspects of green tribology such as the concept, role and goal, principles, focus areas, challenges, “zero-wear” effect were considered in details.
\nThe concept, role and goal of green tribology were clarified. Green tribology can be defined as an interdisciplinary field attributed to the broad induction of various concepts such as energy, materials science, green lubrication, and environmental science. The goal and essence of green tribology is to save material resources, improve energy efficiency, decrease emissions, shock absorption, investigate and apply novel natural bio- and eco-lubricants as well as to reduce the harmful effects of technical systems on the environment, and consequently, improve the quality of human life.
\nThe twelve principles and three areas of green tribology were analyzed. Observation of these principles can greatly reduce the environmental impact of tribological processes, assist economic development and, consequently, improve the quality of life. The integration of these areas remains the major challenge of green tribology and defines the future directions of research in this field.
\nWithin the framework of this work, one of the most important tribological effects, which is exclusively the basis for green tribology - the “zero-wear” effect in friction (selective transfer effect) was discussed.
\nAs a result, this work allows us to conclude that green tribology is an environmentally friendly and energy-saving concept and, moreover, there are many opportunities for its inclusion in a sustainable society on a global scale. Furthermore, there is a need for tribologists to collaborate towards the development and application of Green tribology.
\nOur gratitude goes to the Institute of Technology and Don State Technical University for supporting this research. The authors also thank the reviewers for carefully reading the chapter and for their constructive comments and suggestions which have improved this paper.
\nThe authors declare that there is no conflict of interest.
Stability constant of the formation of metal complexes is used to measure interaction strength of reagents. From this process, metal ion and ligand interaction formed the two types of metal complexes; one is supramolecular complexes known as host-guest complexes [1] and the other is anion-containing complexes. In the solution it provides and calculates the required information about the concentration of metal complexes.
Solubility, light, absorption conductance, partitioning behavior, conductance, and chemical reactivity are the complex characteristics which are different from their components. It is determined by various numerical and graphical methods which calculate the equilibrium constants. This is based on or related to a quantity, and this is called the complex formation function.
During the displacement process at the time of metal complex formation, some ions disappear and form a bonding between metal ions and ligands. It may be considered due to displacement of a proton from a ligand species or ions or molecules causing a drop in the pH values of the solution [2]. Irving and Rossotti developed a technique for the calculation of stability constant, and it is called potentiometric technique.
To determine the stability constant, Bjerrum has used a very simple method, and that is metal salt solubility method. For the studies of a larger different variety of polycarboxylic acid-, oxime-, phenol-containing metal complexes, Martel and Calvin used the potentiometric technique for calculating the stability constant. Those ligands [3, 4] which are uncharged are also examined, and their stability constant calculations are determined by the limitations inherent in the ligand solubility method. The limitations of the metal salt solubility method and the result of solubility methods are compared with this. M-L, MLM, and (M3) L are some types of examples of metal-ligand bonding. One thing is common, and that is these entire types metal complexes all have one ligand.
The solubility method can only usefully be applied to studies of such complexes, and it is best applied for ML; in such types of system, only ML is formed. Jacqueline Gonzalez and his co-worker propose to explore the coordination chemistry of calcium complexes. Jacqueline and et al. followed this technique for evaluate the as partial model of the manganese-calcium cluster and spectrophotometric studies of metal complexes, i.e., they were carried calcium(II)-1,4-butanediamine in acetonitrile and calcium(II)-1,2-ethylendiamine, calcium(II)-1,3-propanediamine by them.
Spectrophotometric programming of HypSpec and received data allows the determination of the formation of solubility constants. The logarithmic values, log β110 = 5.25 for calcium(II)-1,3-propanediamine, log β110 = 4.072 for calcium(II)-1,4-butanediamine, and log β110 = 4.69 for calcium(II)-1,2-ethylendiamine, are obtained for the formation constants [5]. The structure of Cimetidine and histamine H2-receptor is a chelating agent. Syed Ahmad Tirmizi has examined Ni(II) cimetidine complex spectrophotometrically and found an absorption peak maximum of 622 nm with respect to different temperatures.
Syed Ahmad Tirmizi have been used to taken 1:2 ratio of metal and cimetidine compound for the formation of metal complex and this satisfied by molar ratio data. The data, 1.40–2.4 × 108, was calculated using the continuous variation method and stability constant at room temperature, and by using the mole ratio method, this value at 40°C was 1.24–2.4 × 108. In the formation of lead(II) metal complexes with 1-(aminomethyl) cyclohexene, Thanavelan et al. found the formation of their binary and ternary complexes. Glycine,
Using the stability constant method, these ternary complexes were found out, and using the parameters such as Δ log K and log X, these ternary complex data were compared with binary complex. The potentiometric technique at room temperature (25°C) was used in the investigation of some binary complex formations by Abdelatty Mohamed Radalla. These binary complexes are formed with 3D transition metal ions like Cu2+, Ni2+, Co2+, and Zn2+ and gallic acid’s importance as a ligand and 0.10 mol dm−3 of NaNO3. Such types of aliphatic dicarboxylic acids are very important biologically. Many acid-base characters and the nature of using metal complexes have been investigated and discussed time to time by researchers [7].
The above acids (gallic and aliphatic dicarboxylic acid) were taken to determine the acidity constants. For the purpose of determining the stability constant, binary and ternary complexes were carried in the aqueous medium using the experimental conditions as stated above. The potentiometric pH-metric titration curves are inferred for the binary complexes and ternary complexes at different ratios, and formation of ternary metal complex formation was in a stepwise manner that provided an easy way to calculate stability constants for the formation of metal complexes.
The values of Δ log K, percentage of relative stabilization (% R. S.), and log X were evaluated and discussed. Now it provides the outline about the various complex species for the formation of different solvents, and using the concentration distribution, these complexes were evaluated and discussed. The conductivity measurements have ascertained for the mode of ternary chelating complexes.
A study by Kathrina and Pekar suggests that pH plays an important role in the formation of metal complexes. When epigallocatechin gallate and gallic acid combine with copper(II) to form metal complexes, the pH changes its speculation. We have been able to determine its pH in frozen and fluid state with the help of multifrequency EPR spectroscopy [8]. With the help of this spectroscopy, it is able to detect that each polyphenol exhibits the formation of three different mononuclear species. If the pH ranges 4–8 for di- or polymeric complex of Cu(II), then it conjectures such metal complexes. It is only at alkaline pH values.
The line width in fluid solutions by molecular motion exhibits an incomplete average of the parameters of anisotropy spin Hamilton. If the complexes are different, then their rotational correlation times for this also vary. The analysis of the LyCEP anisotropy of the fluid solution spectra is performed using the parameters determined by the simulation of the rigid boundary spectra. Its result suggests that pH increases its value by affecting its molecular mass. It is a polyphenol ligand complex with copper, showing the coordination of an increasing number of its molecules or increasing participation of polyphenol dimers used as ligands in the copper coordination region.
The study by Vishenkova and his co-worker [8] provides the investigation of electrochemical properties of triphenylmethane dyes using a voltammetric method with constant-current potential sweep. Malachite green (MG) and basic fuchsin (BF) have been chosen as representatives of the triphenylmethane dyes [9]. The electrochemical behavior of MG and BF on the surface of a mercury film electrode depending on pH, the nature of background electrolyte, and scan rate of potential sweep has been investigated.
Using a voltammetric method with a constant-current potential sweep examines the electrical properties of triphenylmethane dye. In order to find out the solution of MG and BF, certain registration conditions have been prescribed for it, which have proved to be quite useful. The reduction peak for the currents of MG and BF has demonstrated that it increases linearly with respect to their concentration as 9.0 × 10−5–7.0 × 10−3 mol/dm3 for MG and 6.0 × 10−5–8.0 × 10−3 mol/dm3 for BF and correlation coefficients of these values are 0.9987 for MG and 0.9961 for BF [10].
5.0 × 10−5 and 2.0 × 10−5 mol/dm3 are the values used as the detection limit of MG and BF, respectively. Stability constants are a very useful technique whose size is huge. Due to its usefulness, it has acquired an umbrella right in the fields of chemistry, biology, and medicine. No science subject is untouched by this. Stability constants of metal complexes are widely used in the various areas like pharmaceuticals as well as biological processes, separation techniques, analytical processes, etc. In the presented chapter, we have tried to explain this in detail by focusing our attention on the applications and solutions of stability of metal complexes in solution.
Stability or formation or binding constant is the type of equilibrium constant used for the formation of metal complexes in the solution. Acutely, stability constant is applicable to measure the strength of interactions between the ligands and metal ions that are involved in complex formation in the solution [11]. A generally these 1-4 equations are expressed as the following ways:
Thus
K1, K2, K3, … Kn are the equilibrium constants and these are also called stepwise stability constants. The formation of the metal-ligand-n complex may also be expressed as equilibrium constants by the following steps:
The parameters K and β are related together, and these are expressed in the following example:
Now the numerator and denominator are multiplied together with the use of [metal-ligand] [metal-ligand2], and after the rearranging we get the following equation:
Now we expressed it as the following:
From the above relation, it is clear that the overall stability constant βn is equal to the product of the successive (i.e., stepwise) stability constants, K1, K2, K3,…Kn. This in other words means that the value of stability constants for a given complex is actually made up of a number of stepwise stability constants. The term stability is used without qualification to mean that the complex exists under a suitable condition and that it is possible to store the complex for an appreciable amount of time. The term stability is commonly used because coordination compounds are stable in one reagent but dissociate or dissolve in the presence of another regent. It is also possible that the term stability can be referred as an action of heat or light or compound. The stability of complex [13] is expressed qualitatively in terms of thermodynamic stability and kinetic stability.
In a chemical reaction, chemical equilibrium is a state in which the concentration of reactants and products does not change over time. Often this condition occurs when the speed of forward reaction becomes the same as the speed of reverse reaction. It is worth noting that the velocities of the forward and backward reaction are not zero at this stage but are equal.
If hydrogen and iodine are kept together in molecular proportions in a closed process vessel at high temperature (500°C), the following action begins:
In this activity, hydrogen iodide is formed by combining hydrogen and iodine, and the amount of hydrogen iodide increases with time. In contrast to this action, if the pure hydrogen iodide gas is heated to 500°C in the reaction, the compound is dissolved by reverse action, which causes hydrogen iodide to dissolve into hydrogen and iodine, and the ratio of these products increases over time. This is expressed in the following reaction:
For the formation of metal chelates, the thermodynamic technique provides a very significant information. Thermodynamics is a very useful technique in distinguishing between enthalpic effects and entropic effects. The bond strengths are totally effected by enthalpic effect, and this does not make any difference in the whole solution in order/disorder. Based on thermodynamics the chelate effect below can be best explained. The change of standard Gibbs free energy for equilibrium constant is response:
Where:
R = gas constant
T = absolute temperature
At 25°C,
ΔG = (− 5.708 kJ mol−1) · log β.
The enthalpy term creates free energy, i.e.,
For metal complexes, thermodynamic stability and kinetic stability are two interpretations of the stability constant in the solution. If reaction moves from reactants to products, it refers to a change in its energy as shown in the above equation. But for the reactivity, kinetic stability is responsible for this system, and this refers to ligand species [14].
Stable and unstable are thermodynamic terms, while labile and inert are kinetic terms. As a rule of thumb, those complexes which react completely within about 1 minute at 25°C are considered labile, and those complexes which take longer time than this to react are considered inert. [Ni(CN)4]2− is thermodynamically stable but kinetically inert because it rapidly exchanges ligands.
The metal complexes [Co(NH3)6]3+ and such types of other complexes are kinetically inert, but these are thermodynamically unstable. We may expect the complex to decompose in the presence of acid immediately because the complex is thermodynamically unstable. The rate is of the order of 1025 for the decomposition in acidic solution. Hence, it is thermodynamically unstable. However, nothing happens to the complex when it is kept in acidic solution for several days. While considering the stability of a complex, always the condition must be specified. Under what condition, the complex which is stable or unstable must be specified such as acidic and also basic condition, temperature, reactant, etc.
A complex may be stable with respect to a particular condition but with respect to another. In brief, a stable complex need not be inert and similarly, and an unstable complex need not be labile. It is the measure of extent of formation or transformation of complex under a given set of conditions at equilibrium [15].
Thermodynamic stability has an important role in determining the bond strength between metal ligands. Some complexes are stable, but as soon as they are introduced into aqueous solution, it is seen that these complexes have an effect on stability and fall apart. For an example, we take the [Co (SCN)4]2+ complex. The ion bond of this complex is very weak and breaks down quickly to form other compounds. But when [Fe(CN)6]3− is dissolved in water, it does not test Fe3+ by any sensitive reagent, which shows that this complex is more stable in aqueous solution. So it is indicated that thermodynamic stability deals with metal-ligand bond energy, stability constant, and other thermodynamic parameters.
This example also suggests that thermodynamic stability refers to the stability and instability of complexes. The measurement of the extent to which one type of species is converted to another species can be determined by thermodynamic stability until equilibrium is achieved. For example, tetracyanonickelate is a thermodynamically stable and kinetic labile complex. But the example of hexa-amine cobalt(III) cation is just the opposite:
Thermodynamics is used to express the difference between stability and inertia. For the stable complex, large positive free energies have been obtained from ΔG0 reaction. The ΔH0, standard enthalpy change for this reaction, is related to the equilibrium constant, βn, by the well thermodynamic equation:
For similar complexes of various ions of the same charge of a particular transition series and particular ligand, ΔS0 values would not differ substantially, and hence a change in ΔH0 value would be related to change in βn values. So the order of values of ΔH0 is also the order of the βn value.
Kinetic stability is referred to the rate of reaction between the metal ions and ligand proceeds at equilibrium or used for the formation of metal complexes. To take a decision for kinetic stability of any complexes, time is a factor which plays an important role for this. It deals between the rate of reaction and what is the mechanism of this metal complex reaction.
As we discuss above in thermodynamic stability, kinetic stability is referred for the complexes at which complex is inert or labile. The term “inert” was used by Tube for the thermally stable complex and for reactive complexes the term ‘labile’ used [16]. The naturally occurring chlorophyll is the example of polydentate ligand. This complex is extremely inert due to exchange of Mg2+ ion in the aqueous media.
The nature of central atom of metal complexes, dimension, its degree of oxidation, electronic structure of these complexes, and so many other properties of complexes are affected by the stability constant. Some of the following factors described are as follows.
In the coordination chemistry, metal complexes are formed by the interaction between metal ions and ligands. For these type of compounds, metal ions are the coordination center, and the ligand or complexing agents are oriented surrounding it. These metal ions mostly are the transition elements. For the determination of stability constant, some important characteristics of these metal complexes may be as given below.
Ligands are oriented around the central metal ions in the metal complexes. The sizes of these metal ions determine the number of ligand species that will be attached or ordinated (dative covalent) in the bond formation. If the sizes of these metal ions are increased, the stability of coordination compound defiantly decreased. Zn(II) metal ions are the central atoms in their complexes, and due to their lower size (0.74A°) as compared to Cd(II) size (0.97A°), metal ions are formed more stable.
Hence, Al3+ ion has the greatest nuclear charge, but its size is the smallest, and the ion N3− has the smallest nuclear charge, and its size is the largest [17]. Inert atoms like neon do not participate in the formation of the covalent or ionic compound, and these atoms are not included in isoelectronic series; hence, it is not easy to measure the radius of this type of atoms.
The properties of stability depend on the size of the metal ion used in the complexes and the total charge thereon. If the size of these metal ions is small and the total charge is high, then their complexes will be more stable. That is, their ratio will depend on the charge/radius. This can be demonstrated through the following reaction:
An ionic charge is the electric charge of an ion which is formed by the gain (negative charge) or loss (positive charge) of one or more electrons from an atom or group of atoms. If we talk about the stability of the coordination compounds, we find that the total charge of their central metal ions affects their stability, so when we change their charge, their stability in a range of constant can be determined by propagating of error [18]. If the charge of the central metal ion is high and the size is small, the stability of the compound is high:
In general, the most stable coordination bonds can cause smaller and highly charged rations to form more stable coordination compounds.
When an electron pair attracts a central ion toward itself, a strong stability complex is formed, and this is due to electron donation from ligand → metal ion. This donation process is increasing the bond stability of metal complexes exerted the polarizing effect on certain metal ions. Li+, Na+, Mg2+, Ca2+, Al3+, etc. are such type of metal cation which is not able to attract so strongly from a highly electronegative containing stable complexes, and these atoms are O, N, F, Au, Hg, Ag, Pd, Pt, and Pb. Such type of ligands that contains P, S, As, Br and I atom are formed stable complex because these accepts electron from M → π-bonding. Hg2+, Pb2+, Cd2+, and Bi3+ metal ions are also electronegative ions which form insoluble salts of metal sulfide which are insoluble in aqueous medium.
Volatile ligands may be lost at higher temperature. This is exemplified by the loss of water by hydrates and ammonia:
The transformation of certain coordination compounds from one to another is shown as follows:
A ligand is an ion or small molecule that binds to a metal atom (in chemistry) or to a biomolecule (in biochemistry) to form a complex, such as the iron-cyanide coordination complex Prussian blue or the iron-containing blood-protein hemoglobin. The ligands are arranged in spectrochemical series which are based on the order of their field strength. It is not possible to form the entire series by studying complexes with a single metal ion; the series has been developed by overlapping different sequences obtained from spectroscopic studies [19]. The order of common ligands according to their increasing ligand field strength is
The above spectrochemical series help us to for determination of strength of ligands. The left last ligand is as weaker ligand. These weaker ligand cannot forcible binding the 3d electron and resultant outer octahedral complexes formed. It is as-
Increasing the oxidation number the value of Δ increased.
Δ increases from top to bottom.
However, when we consider the metal ion, the following two useful trends are observed:
Δ increases with increasing oxidation number.
Δ increases down a group. For the determination of stability constant, the nature of the ligand plays an important role.
The following factors described the nature of ligands.
The size and charge are two factors that affect the production of metal complexes. The less charges and small sizes of ligands are more favorable for less stable bond formation with metal and ligand. But if this condition just opposite the product of metal and ligand will be a more stable compound. So, less nuclear charge and more size= less stable complex whereas if more nuclear charge and small in size= less stable complex. We take fluoride as an example because due to their smaller size than other halide and their highest electro negativity than the other halides formed more stable complexes. So, fluoride ion complexes are more stable than the other halides:
As compared to S2− ion, O22− ions formed more stable complexes.
It is suggested by Calvin and Wilson that the metal complexes will be more stable if the basic character or strength of ligands is higher. It means that the donating power of ligands to central metal ions is high [20].
It means that the donating power of ligands to central metal ions is high. In the case of complex formation of aliphatic diamines and aromatic diamines, the stable complex is formed by aliphatic diamines, while an unstable coordination complex is formed with aromatic diamines. So, from the above discussion, we find that the stability will be grater if the e-donation power is greater.
Thus it is clear that greater basic power of electron-donating species will form always a stable complex. NH3, CN−, and F− behaved as ligands and formed stable complexes; on the other hand, these are more basic in nature.
We know that if the concentration of coordination group is higher, these coordination compounds will exist in the water as solution. It is noted that greater coordinating tendency show the water molecules than the coordinating group which is originally present. SCN− (thiocynate) ions are present in higher concentration; with the Co2+ metal ion, it formed a blue-colored complex which is stable in state, but on dilution of water medium, a pink color is generated in place of blue, or blue color complex is destroyed by [Co(H2O)6]2+, and now if we added further SCN−, the pink color will not appear:
Now it is clear that H2O and SCN− are in competition for the formation of Co(II) metal-containing complex compound. In the case of tetra-amine cupric sulfate metal complex, ammonia acts as a donor atom or ligand. If the concentration of NH3 is lower in the reaction, copper hydroxide is formed but at higher concentration formed tetra-amine cupric sulfate as in the following reaction:
For a metal ion, chelating ligand is enhanced and affinity it and this is known as chelate effect and compared it with non-chelating and monodentate ligand or the multidentate ligand is acts as chelating agent. Ethylenediamine is a simple chelating agent (Figure 1).
Structure of ethylenediamine.
Due to the bidentate nature of ethylenediamine, it forms two bonds with metal ion or central atom. Water forms a complex with Ni(II) metal ion, but due to its monodentate nature, it is not a chelating ligand (Figures 2 and 3).
Structure of chelating configuration of ethylenediamine ligand.
Structure of chelate with three ethylenediamine ligands.
The dentate cheater of ligand provides bonding strength to the metal ion or central atom, and as the number of dentate increased, the tightness also increased. This phenomenon is known as chelating effect, whereas the formation of metal complexes with these chelating ligands is called chelation:
or
Some factors are of much importance for chelation as follows.
The sizes of the chelating ring are increased as well as the stability of metal complex decreased. According to Schwarzenbach, connecting bridges form the chelating rings. The elongated ring predominates when long bridges connect to the ligand to form a long ring. It is usually observed that an increased a chelate ring size leads to a decrease in complex stability.
He interpreted this statement. The entropy of complex will be change if the size of chelating ring is increased, i.e., second donor atom is allowed by the chelating ring. As the size of chelating ring increased, the stability should be increased with entropy effect. Four-membered ring compounds are unstable, whereas five-membered are more stable. So the chelating ring increased its size and the stability of the formed metal complexes.
The number of chelating rings also decides the stability of complexes. Non-chelating metal compounds are less stable than chelating compounds. These numbers increase the thermodynamic volume, and this is also known as an entropy term. In recent years ligands capable of occupying as many as six coordination positions on a single metal ion have been described. The studies on the formation constants of coordination compounds with these ligands have been reported. The numbers of ligand or chelating agents are affecting the stability of metal complexes so as these numbers go up and down, the stability will also vary with it.
For the Ni(II) complexes with ethylenediamine as chelating agent, its log K1 value is 7.9 and if chelating agents are trine and penten, then the log K1 values are 7.9 and 19.3, respectively. If the metal ion change Zn is used in place of Ni (II), then the values of log K1 for ethylenediamine, trine, and penten are 6.0, 12.1, and 16.2, respectively. The log βMY values of metal ions are given in Table 1.
Metal ion | log βMY (25°C, I = 0.1 M) |
---|---|
Ca2+ | 11.2 |
Cu2+ | 19.8 |
Fe3+ | 24.9 |
Metal ion vs. log βMY values.
Ni(NH3)62+ is an octahedral metal complex, and at 25 °C its log β6 value is 8.3, but Ni(ethylenediamine)32+ complex is also octahedral in geometry, with 18.4 as the value of log β6. The calculated stability value of Ni(ethylenediamine)32+ 1010 times is more stable because three rings are formed as chelating rings by ethylenediamine as compared to no such ring is formed. Ethylenediaminetetraacetate (EDTA) is a hexadentate ligand that usually formed stable metal complexes due to its chelating power.
A special effect in molecules is when the atoms occupy space. This is called steric effect. Energy is needed to bring these atoms closer to each other. These electrons run away from near atoms. There can be many ways of generating it. We know the repulsion between valence electrons as the steric effect which increases the energy of the current system [21]. Favorable or unfavorable any response is created.
For example, if the static effect is greater than that of a product in a metal complex formation process, then the static increase would favor this reaction. But if the case is opposite, the skepticism will be toward retardation.
This effect will mainly depend on the conformational states, and the minimum steric interaction theory can also be considered. The effect of secondary steric is seen on receptor binding produced by an alternative such as:
Reduced access to a critical group.
Stick barrier.
Electronic resonance substitution bond by repulsion.
Population of a conformer changes due to active shielding effect.
The macrocyclic effect is exactly like the image of the chelate effect. It means the principle of both is the same. But the macrocyclic effect suggests cyclic deformation of the ligand. Macrocyclic ligands are more tainted than chelating agents. Rather, their compounds are more stable due to their cyclically constrained constriction. It requires some entropy in the body to react with the metal ion. For example, for a tetradentate cyclic ligand, we can use heme-B which forms a metal complex using Fe+2 ions in biological systems (Figure 4).
Structure of hemoglobin is the biological complex compound which contains Fe(II) metal ion.
The n-dentate chelating agents play an important role for the formation of more stable metal complexes as compared to n-unidentate ligands. But the n-dentate macrocyclic ligand gives more stable environment in the metal complexes as compared to open-chain ligands. This change is very favorable for entropy (ΔS) and enthalpy (ΔH) change.
There are so many parameters to determination of formation constants or stability constant in solution for all types of chelating agents. These numerous parameters or techniques are refractive index, conductance, temperature, distribution coefficients, refractive index, nuclear magnetic resonance volume changes, and optical activity.
Solubility products are helpful and used for the insoluble salt that metal ions formed and complexes which are also formed by metal ions and are more soluble. The formation constant is observed in presence of donor atoms by measuring increased solubility.
To determine the solubility constant, it involves the distribution of the ligands or any complex species; metal ions are present in two immiscible solvents like water and carbon tetrachloride, benzene, etc.
In this method metal ions or ligands are present in solution and on exchanger. A solid polymers containing with positive and negative ions are ion exchange resins. These are insoluble in nature. This technique is helpful to determine the metal ions in resin phase, liquid phase, or even in radioactive metal. This method is also helpful to determine the polarizing effect of metal ions on the stability of ligands like Cu(II) and Zn(II) with amino acid complex formation.
At the equilibrium free metal and ions are present in the solution, and using the different electrometric techniques as described determines its stability constant.
This method is based upon the titration method or follows its principle. A stranded acid-base solution used as titrate and which is titrated, it may be strong base or strong acid follows as potentiometrically. The concentration of solution using 103− M does not decomposed during the reaction process, and this method is useful for protonated and nonprotonated ligands.
This is the graphic method used to determine the stability constant in producing metal complex formation by plotting a polarograph between the absences of substances and the presence of substances. During the complex formation, the presence of metal ions produced a shift in the half-wave potential in the solution.
If a complex is relatively slow to form and also decomposes at measurable rate, it is possible, in favorable situations, to determine the equilibrium constant.
This involves the study of the equilibrium constant of slow complex formation reactions. The use of tracer technique is extremely useful for determining the concentrations of dissociation products of the coordination compound.
This method is based on the study of the effect of an equilibrium concentration of some ions on the function at a definite organ of a living organism. The equilibrium concentration of the ion studied may be determined by the action of this organ in systems with complex formation.
The solution of 25 ml is adopted by preparing at the 1.0 × 10−5 M ligand or 1.0 × 10−5 M concentration and 1.0 × 10−5 M for the metal ion:
The solutions containing the metal ions were considered both at a pH sufficiently high to give almost complete complexation and at a pH value selected in order to obtain an equilibrium system of ligand and complexes.
In order to avoid modification of the spectral behavior of the ligand due to pH variations, it has been verified that the range of pH considered in all cases does not affect absorbance values. Use the collected pH values adopted for the determinations as well as selected wavelengths. The ionic strengths calculated from the composition of solutions allowed activity coefficient corrections. Absorbance values were determined at wavelengths in the range 430–700 nm, every 2 nm.
For a successive metal complex formation, use this method. If ligand is protonate and the produced complex has maximum number of donate atoms of ligands, a selective light is absorbed by this complex, while for determination of stability constant, it is just known about the composition of formed species.
Bjerrum (1941) used the method stepwise addition of the ligands to coordination sphere for the formation of complex. So, complex metal–ligand-n forms as the following steps [22]. The equilibrium constants, K1, K2, K3, … Kn are called stepwise stability constants. The formation of the complex metal-ligandn may also be expressed by the following steps and equilibrium constants.
Where:
M = central metal cation
L = monodentate ligand
N = maximum coordination number for the metal ion M for the ligand
If a complex ion is slow to reach equilibrium, it is often possible to apply the method of isotopic dilution to determine the equilibrium concentration of one or more of the species. Most often radioactive isotopes are used.
This method was extensively used by Werner and others to study metal complexes. In the case of a series of complexes of Co(III) and Pt(IV), Werner assigned the correct formulae on the basis of their molar conductance values measured in freshly prepared dilute solutions. In some cases, the conductance of the solution increased with time due to a chemical change, e.g.,
It is concluded that the information presented is very important to determine the stability constant of the ligand metal complexes. Some methods like spectrophotometric method, Bjerrum’s method, distribution method, ion exchange method, electrometric techniques, and potentiometric method have a huge contribution in quantitative analysis by easily finding the stability constants of metal complexes in aqueous solutions.
All the authors thank the Library of University of Delhi for reference books, journals, etc. which helped us a lot in reviewing the chapter.
.
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