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This book focuses on the chemistry and processes for conversion and utilization of carbon dioxide. Topics include CO 2 utilization, its conversion to industrial chemicals and fuels, its coversion via synthesis gas, and new catalysts and chemical processes for conversion.
The use of fossil fuels to meet our energy requirements has contributed significantly to increase the atmospheric carbon dioxide level causing global warming. This calls for the development of processes to reduce CO2 level and its conversion to other value-added products. In this regard, photocatalytic CO2 reduction using sunlight is a key reaction to achieve artificial photosynthesis to produce solar or renewable fuels. Designing efficient and robust catalysts for this reduction reaction is crucial and remains a challenging task. Recently, N-heterocyclic carbenes (NHCs) have emerged as strong donor ligands that are useful for forming transition metal-based catalysts. The combination of two NHCs with a central pyridyl ring in a symmetric fashion results in a tridentate CNC-pincer framework that can promote catalyst stability. Metal complexes containing such CNC-pincer ligands along with other co-ligands have been synthesized, characterized, and evaluated for photocatalytic CO2 reduction reaction (CO2-RR). We have shown that the use of a bidentate co-ligand (2,2ʣ-bipyiridine (bpy)) along with a CNC-pincer in ruthenium complexes ([(CNC)RuIIL(bpy)]n+, L is chloride or acetonitrile) resulted in the development of self-sensitized catalysts for photocatalytic CO2-RR under photosensitizer (PS) free conditions. The effect of various donor groups at the 4-position of the central pyridyl ring in CNC-pincer ligand has been evaluated via structure-activity relationships for sensitized photocatalytic CO2-RR in the presence of an external PS using [(CNC)RuIICl(MeCN)2]+ complexes. We have also compared the positional effect for one of the donor group. To further explore the structure-activity relationships, 11 novel ruthenium complexes with the general formula [(CNC)RuIIL(NN)]n+ (NN = diimine ligands, L = chloride or bromide or acetonitrile) were synthesized, characterized, and evaluated for sensitized and self-sensitized photocatalytic CO2-RR. The structures include two CNC-pincer ligands based on imidazole and benzimidazole derived NHCs and three diimine ligands including bpy, 4,4ʣ-dimethyl-2,2ʣ-bipyridine (dmb), and 1,10-phenanthroline. The development of heterogeneous catalysts has also been pursued. Two highly active homogeneous photocatalysts containing CNC-pincer and bpy co-ligand on ruthenium were considered for surface immobilization to develop heterogeneous catalysts with well-defined active sites. Syntheses of ruthenium complexes via bpy ligand modifications are described that can be immobilized onto an inert solid support for surface organometallic chemistry (SOMC). In addition, we have attempted to explore the use of first-row transition metals to develop catalysts for photocatalytic CO2-RR. The development of nickel CNC-pincer complexes for this reduction reaction has been described. We also aimed to synthesized iron-based catalysts and the efforts are described. The use of bulkier wing-tip groups on the CNC-pincer ligands and phosphine co-ligand resulted in the formation of miscellaneous ruthenium complexes.
Explore green catalytic reactions with this reference from a renowned leader in the field Green reactions—like photo-, photoelectro-, and electro-catalytic reactions—offer viable technologies to solve difficult problems without significant damage to the environment. In particular, some gas-involved reactions are especially useful in the creation of liquid fuels and cost-effective products. In Photo- and Electro-Catalytic Processes: Water Splitting, N2 Fixing, CO2 Reduction, award-winning researcher Jianmin Ma delivers a comprehensive overview of photo-, electro-, and photoelectron-catalysts in a variety of processes, including O2 reduction, CO2 reduction, N2 reduction, H2 production, water oxidation, oxygen evolution, and hydrogen evolution. The book offers detailed information on the underlying mechanisms, costs, and synthetic methods of catalysts. Filled with authoritative and critical information on green catalytic processes that promise to answer many of our most pressing energy and environmental questions, this book also includes: Thorough introductions to electrocatalytic oxygen reduction and evolution reactions, as well as electrocatalytic hydrogen evolution reactions Comprehensive explorations of electrocatalytic water splitting, CO2 reduction, and N2 reduction Practical discussions of photoelectrocatalytic H2 production, water splitting, and CO2 reduction In-depth examinations of photoelectrochemical oxygen evolution and nitrogen reduction Perfect for catalytic chemists and photochemists, Photo- and Electro-Catalytic Processes: Water Splitting, N2 Fixing, CO2 Reduction also belongs in the libraries of materials scientists and inorganic chemists seeking a one-stop resource on the novel aspects of photo-, electro-, and photoelectro-catalytic reactions.
In chemistry, photocatalysis refers to the acceleration of a photoreaction in the presence of a catalyst. Various aspects and applications of this process are described in the six chapters of this book. Chapter One addresses the reduction and oxidation of heavy metals by the photocatalytic process to produce less toxic forms, thus reducing pollution. Chapter Two reviews some issues of photocatalytic reactions which may have been overlooked in other reports. Chapter Three deals with the utilisation of ZnO-CdO nanoblocks as adsorbent and efficient solar photocatalysts towards brilliant cresol blue degradation. Chapter Four explains heterogeneous photocatalysis through the use of titanium and tungsten oxide nanostructures. Chapter Five reports the fabrication and evaluation of TiO2 nanowires supported on graphene and sensitised with Ag in a unique hierarchical three-dimensional sandwich structure. Lastly, Chapter Six provides an overview of recent achievements in C-N bond formation reactions triggered by visible light-induced DDQ-photoredox catalysis.
This book comprises a detailed overview on the role of photocatalysts for environmental remediation, hydrogen production and carbon dioxide reduction. Effective ways to enhance the photocatalytic activity of the material via doping, hybrid material, laser light and nanocomposites have been discussed in this book. The book also further elaborates the role of metal nanoparticles, rare earth doping, sensitizers, surface oxygen vacancy, interface engineering and band gap engineering for enhancing the photocatalytic activity. An approach to recover the photocatalytic material via immobilization is also presented. This book brings to light much of the recent research in the development of such semiconductor photocatalytic systems. The book will thus be of relevance to researchers in the field of: material science, environmental science & technology, photocatalytic applications, newer methods of energy generation & conversion and industrial applications.
CO2 Conversion and Utilization Comprehensive overview of current development of various catalysts in CO2 conversion and utilization through photocatalytic and electrochemical methods CO2 Conversion and Utilization systematically summarizes the development of CO2 photo- and electro-conversion and utilization, especially the reaction mechanism, engineering and technology of testing, and preparation methods and physicochemical properties of various catalytic materials. The rational design and preparation of catalysts, development of characterization technologies, and in-depth understanding of catalytic mechanisms are systematically discussed. In particular, the various parameters influencing the photocatalytic and electrochemical CO2 reduction are emphasized. The underlying challenges and perspectives for the future development of efficient catalysts for CO2 reduction to specific chemicals and fuels are discussed at the end of the text. Written by a highly qualified author with significant experience in the field, CO2 Conversion and Utilization includes information on: Measurement systems and parameters for CO2 photo/electro-conversion, CO2 photo/electro-conversion mechanism, and Cu-based and Cu-free metal materials for electrocatalytic CO2 reduction Organic-inorganic, metal organic framework, and covalent organic framework hybrid materials for CO2 photo/electro-conversion Single/dual-atom catalysts, homogeneous catalysts, and high-entropy alloys for CO2 photo/electro-conversion Semiconductor composite and carbon-based materials for photocatalytic CO2 reduction, novel routes for CO2 utilization via metal-CO2 batteries, and CO2 conversion into long-chain compounds Providing comprehensive coverage of the subject, CO2 Conversion and Utilization is of high interest for scientific researchers as well as engineers and technicians in industry, including but not limited to photochemists, electrochemists, environmental chemists, catalytic chemists, chemists in industry, and inorganic chemists.
Presenting the basic science of semiconductor photocatalysis together with the various practical applications, this textbook is ideal for graduate students. It covers fundamental principles and applicable techniques of light, solid state physics, electrochemistry, reaction kinetics, and materials processing. A solid understanding of semiconductor photoelectrochemistry is developed through discussing the basic properties of a representative photocatalytic material, TiO2; the basic science of the light absorption phenomenon and the application to the powder suspension useful for the photocatalytic research; and the electronic state of semiconductors. Following this, the textbook moves on to explore photoelectrochemistry; the mechanism and kinetic analysis of photocatalytic reactions; typical fabrication methods of common photocatalysts and the factors for improving photocatalytic activity; and evaluation methods of photocatalytic activity. The textbook concludes by looking at the future prospects of the applications of photocatalysis. This introductory textbook provides a foundation in photocatalysis to supplement graduate courses in catalysis, environmental science, materials science and chemical engineering.
Photocatalysis, reactions carried out in the presence of a semiconductor and light, is rapidly becoming one of the most active areas of chemical research, with applications in areas such as electrochemistry, medicine, and environmental chemistry, Photocatalysis: Principles and Applications stresses the development of various types of photocatalytic semiconductors, including binary, ternary, quaternary, and composite, and their modifications by metallization, sensitization, and doping to enhance their photocatalytic activities. In addition to describing the principles and mechanisms of photocatalysis, it also discusses other possible applications of photocatalysis such as use as antifouling agents, controlling air pollution by degrading contaminants present in the environment, self-cleaning of glasses and tiles in the presence of light/artificial light, green composites, wastewater treatment, hydrogen generation, and inactivation of microorganisms. The book also describes medical applications and summarizes efforts in the field of photosplitting of water as a newer energy source and photoreduction of carbon dioxide for providing synthetic fuels and also a step towards mimicking photosynthesis. Introduces the basic principle of photocatalysis. Provides an overview of the types of semiconductors, their immobilization, and modifications to make them more active. Gives possible applications of photocatalysis in wastewater treatment and strategy to combat against different kinds of pollutions like water, air, and soil. Summarizes efforts in the field of photosplitting of water as a newer energy source and photoreduction of carbon dioxide for providing synthetic fuels and as a step towards mimicking photosynthesis. Discusses inactivation of different kinds of microorganisms. Covers medical applications. Features Introduces the basic principle of photocatalysis. Provides an overview of the types of semiconductors, their immobilization, and modifications to make them more active. Gives possible applications of photocatalysis in wastewater treatment and strategy to combat against different kinds of pollutions like water, air, and soil. Summarizes efforts in the field of photosplitting of water as a newer energy source and photoreduction of carbon dioxide for providing synthetic fuels and as a step towards mimicking photosynthesis. Discusses inactivation of different kinds of microorganisms. Covers medical applications.
This book describes the photocatalytic mechanism, factors affecting photocatalytic activity, design and preparation of different kinds of nanostructured photocatalysts, and their applications in the environmental and energy fields. Further, it illustrates a broad range of modification methods including ion-doping, heterojunction, noble metal deposition, morphological control and sensitizations, which are used to extend the light absorption range of photocatalysts and reduce recombination between electrons and holes. Promising applications include water splitting, contaminant decomposition and photocatalytic reduction of CO2, which are closely related to environmental redemption and new energy development. The book offers an intriguing and useful guide for a broad readership in various fields of catalysis, material sciences, environment and energy.
The solar-light driven photocatalysis is considered a promising solution to both energy-shortage and environmental issues. In photocatalysis, a semiconductor-based photocatalyst is key to efficient CO2 reduction. Among others, graphitic carbon nitride and quantum dots materials are the most investigated because of their easy synthesis, low cost, and outstanding physicochemical properties. Numerous g-C3N4 and quantum dots - based nanostructured photocatalysts have been developed and studied for photocatalytic CO2 reduction. However, their photocatalytic performance is still moderate due to the rapid charge recombination and insufficient solar-light absorption. This thesis employed facile and new strategies to develop three efficient photocatalysts for CO2 reduction. The synthesized materials exhibit unique structural properties with improved solar-light absorption and increased charge separation rate, thus contributing to photocatalytic efficiency. For the g-C3N4 materials, we first employed cobalt cluster embedded graphitic carbon nitride as a cocatalyst for CO2 reduction by copolymerization between urea and cobalt complex as g-C3N4 and cobalt cluster precursors, respectively. Using 4,4'-Diamino-2,2'-bipyridine as a coordinating ligand of the cobalt complex is beneficial. First, it can copolymerize with urea during the thermolysis for the g-C3N4 formation, thus improving solar-light absorption of g-C3N4. Secondly, it can stabilize the cobalt cluster and provide and efficient electron transfer pathway between g-C3N4 and the cobalt cluster, resulting in enhanced photocatalytic performance. In the second material, we attempted to improve the solar-light absorption of g-C3N4 by incorporating TiN plasmonic nanoparticles onto the surface of g-C3N4 nanosheets. Before the incorporation, the surface of plasmonic TiN nanoparticles is grafted with amino groups to enhance the interaction with urea during the thermal copolymerization process. The synthesized material exhibited enhanced solar-light absorption and improved charge separation. As a result, this photocatalyst demonstrated high performance for photocatalytic CO2 reduction under solar-light irradiation. Regarding quantum dots material, we attempted to explore the relationship between the localized protons near the active sites and the photocatalytic performance by employing 3- mercaptopropionate as a proton shutter on CdS quantum dot surfaces. A facile aqueous synthesis was utilized to synthesize the water-soluble 3-mercaptopropionic acid (MPA)- capped CdS quantum dots. It was found that the enhanced photocatalytic activity of functional CdS quantum dots could be attributed to the cooperative interaction between localized protons and surface Cd atoms, which behave as a result of the Lewis acid and Lewis base interaction, respectively.