Well-defined Nanoparticle Electrocatalysts for the Carbon Dioxide and Oxygen Reduction Reactions

Well-defined Nanoparticle Electrocatalysts for the Carbon Dioxide and Oxygen Reduction Reactions PDF Author: Jamie Allyce Trindell
Publisher:
ISBN:
Category :
Languages : en
Pages : 398

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Book Description
The lack of structurally diverse electrocatalysts having high activity and controlled selectivity has limited progress in the development of technologically relevant electrochemical transformations. The key to making progress is the synergy between experiment and theory, and particularly experimental model systems against which the efficacy of theory can be benchmarked. The goal of this dissertation is to address the persisting experimental limitations that erode the fruitfulness of this union between theory and electrocatalysis. To this end, well-defined nanoparticle electrocatalysts enabling experimental validation of theoretical predictions are reported here for the carbon dioxide and oxygen reduction reactions, respectively. First, we describe the use of ex-situ scanning transmission electron microscopy (STEM) to analyze the growth of gold nanoparticles (AuNPs) during electrocatalytic CO2 reduction (Chapter 2). Relative to citrate-capped AuNPs, dendrimer-encapsulated Au NPs (Au DENs) demonstrate significantly improved structural stability during CO2 electrolysis. This work highlights the importance of performing catalyst characterization both before and after (and, ideally, during) electrochemical measurements to identify the most accurate computational models for a given electrocatalytic system. Next, we focus on Pd-based nanoalloy catalysts for the oxygen reduction reaction (ORR). Chapter 3 details the experimental verification of PdIr nanoalloy catalysts predicted to have worse catalytic activity towards the oxygen reduction reaction (ORR) than their monometallic counterparts. Specifically, alloying Ir with Pd systematically decreases the ORR activity relative to monometallic Pd NPs. The findings of this study are significant because verifying the ability of theoretical predictions to both rule-in and rule-out potential catalysts holds the key for allowing theory to guide catalyst design. Chapter 4 reports experimental evidence of composition-dependent modulation of O-binding energies on Au [subscript x] Pd [subscript (300-x)] DENs. Specifically, electrochemical characterization identifies unique active sites on AuPd nanoalloys. The concept of surface ensembles, or the presence of unique active sites on the surface of nanoalloys, is a useful concept in theoretical models that is lacking in experimental verification. Altogether, the work described in this dissertation aims to continue to close the gap between theory and experiment in the field of electrocatalysis

Well-defined Nanoparticle Electrocatalysts for the Carbon Dioxide and Oxygen Reduction Reactions

Well-defined Nanoparticle Electrocatalysts for the Carbon Dioxide and Oxygen Reduction Reactions PDF Author: Jamie Allyce Trindell
Publisher:
ISBN:
Category :
Languages : en
Pages : 398

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Book Description
The lack of structurally diverse electrocatalysts having high activity and controlled selectivity has limited progress in the development of technologically relevant electrochemical transformations. The key to making progress is the synergy between experiment and theory, and particularly experimental model systems against which the efficacy of theory can be benchmarked. The goal of this dissertation is to address the persisting experimental limitations that erode the fruitfulness of this union between theory and electrocatalysis. To this end, well-defined nanoparticle electrocatalysts enabling experimental validation of theoretical predictions are reported here for the carbon dioxide and oxygen reduction reactions, respectively. First, we describe the use of ex-situ scanning transmission electron microscopy (STEM) to analyze the growth of gold nanoparticles (AuNPs) during electrocatalytic CO2 reduction (Chapter 2). Relative to citrate-capped AuNPs, dendrimer-encapsulated Au NPs (Au DENs) demonstrate significantly improved structural stability during CO2 electrolysis. This work highlights the importance of performing catalyst characterization both before and after (and, ideally, during) electrochemical measurements to identify the most accurate computational models for a given electrocatalytic system. Next, we focus on Pd-based nanoalloy catalysts for the oxygen reduction reaction (ORR). Chapter 3 details the experimental verification of PdIr nanoalloy catalysts predicted to have worse catalytic activity towards the oxygen reduction reaction (ORR) than their monometallic counterparts. Specifically, alloying Ir with Pd systematically decreases the ORR activity relative to monometallic Pd NPs. The findings of this study are significant because verifying the ability of theoretical predictions to both rule-in and rule-out potential catalysts holds the key for allowing theory to guide catalyst design. Chapter 4 reports experimental evidence of composition-dependent modulation of O-binding energies on Au [subscript x] Pd [subscript (300-x)] DENs. Specifically, electrochemical characterization identifies unique active sites on AuPd nanoalloys. The concept of surface ensembles, or the presence of unique active sites on the surface of nanoalloys, is a useful concept in theoretical models that is lacking in experimental verification. Altogether, the work described in this dissertation aims to continue to close the gap between theory and experiment in the field of electrocatalysis

Oxygen Reduction Reactions

Oxygen Reduction Reactions PDF Author: P. Kulesza
Publisher: The Electrochemical Society
ISBN: 1607686163
Category : Science
Languages : en
Pages : 51

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Book Description


Surface-Enhanced Raman Scattering

Surface-Enhanced Raman Scattering PDF Author: Zhong-Qun Tian
Publisher: John Wiley & Sons Incorporated
ISBN: 9780470068083
Category : Science
Languages : en
Pages : 400

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Book Description
Surface-Enhanced Raman Spectroscopy: Principles, Experiments, and Applications is a comprehensive, up to date, and balanced treatment of the theoretical and practical aspects of Surface-Enhanced Raman Scattering (SERS), a useful branch of spectroscopy for several areas of science. This book describes the basic principles of SERS, including SERS mechanisms, performing SERS measurements, and interpreting data. Also emphasized are applications in electrochemistry; catalysis; surface processing and corrosion; Self-Assemble-Layer and L-B Films; polymer science; biology; medicine and drug analysis; sensors; fuel cells; forensics; and archaeology. It is an essential guide for student and professional analytical chemists.

Electrocatalytic Reduction of Oxygen and Oxidation of Carbon Monoxide on Metal Oxide Thin Film Supported Metal Nanoparticles

Electrocatalytic Reduction of Oxygen and Oxidation of Carbon Monoxide on Metal Oxide Thin Film Supported Metal Nanoparticles PDF Author: Aigerim Galyamova
Publisher:
ISBN:
Category :
Languages : en
Pages : 0

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Book Description
In this work, we use a well-defined model for studying electrocatalytic reactions at metal nanoparticles (NPs) in contact with metal oxide thin films using the synergy between predictive theory and confirming experiments. The goal of this work is to build an in-depth understanding of strong metal-support interactions (SMSI) and their effect on electrocatalytic reactions that are of critical importance for the production and use of chemical fuels. These reactions are electrocatalytic reduction of oxygen (ORR) and oxidation of carbon monoxide (CO). The work described herein uses a robust experimental model that allows us to study SMSI and their effect on electrocatalytic reactions in the absence and presence of direct contact between NP and metal oxide thin film. We started by using a theory-first approach in which density functional theory (DFT) predicted enhanced ORR activity on AuNPs supported on TiO2(110). The experimental results were in quantitative agreement with DFT, where we observed a positive shift in ORR onset potential and a change in the number of effective electrons transferred when Au147 NPs were in direct contact with TiO [subscript x] (x = 1.9 or 2.0) thin film compared to when the support interactions were absent. We wished to expand the complexity of the theory required for comparison to experiments. Hence, we chose to investigate the CO electrooxidation reaction, which requires two descriptors rather than the single descriptor used for the ORR for DFT analysis. Accordingly, we experimentally studied the effects of TiO [subscript x] (x = 1.9 or 2.0) thin film supports on the electrocatalytic activity of Au147 NPs or Pt55 NPs towards the CO electrooxidation reaction. Finally, we further expanded our understanding of SMSI by shifting our focus from oxygen vacancy to metal vacancy containing metal oxide thin films. We experimentally studied the effects of Ni0.9O thin film supports on the electrocatalytic activity of PtNPs towards the CO electrooxidation reaction. We observed a negative shift in CO oxidation peak potential when PtNPs were in contact with Ni0.9O thin films compared to when support interactions were absent. The experimentally observed results were validated with first principle theory calculations

Non-Noble Metal Fuel Cell Catalysts

Non-Noble Metal Fuel Cell Catalysts PDF Author: Zhongwei Chen
Publisher: John Wiley & Sons
ISBN: 9783527333240
Category : Technology & Engineering
Languages : en
Pages : 0

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Book Description
Written and edited by top fuel cell catalyst scientists and engineers from both industry and academia, this is the first book to provide a complete overview of this hot topic. It covers the synthesis, characterization, activity validation and modeling of different non-noble metal electrocatalysts, as well as their integration into fuel cells and their performance validation, while also discussing those factors that will drive fuel cell commercialization. With its well-structured approach, this is a must-have for researchers working on the topic, and an equally valuable companion for newcomers to the field.

Nano-electrocatalyst for Oxygen Reduction Reaction

Nano-electrocatalyst for Oxygen Reduction Reaction PDF Author: Omar Solorza Feria
Publisher: CRC Press
ISBN: 1040043496
Category : Science
Languages : en
Pages : 350

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Book Description
Global warming switches our reliance from fossil fuels to green, sustainable renewable energy sources. Because of its promising nature, high-efficiency nano-electrocatalysts have sparked interest in renewable energy. Hydrogen fuel cell/polymer electrolyte membrane (PEM) vehicles are the most environmentally conscious electromobility vehicles, with a high energy density and quick refuelling technology, prompting the auto industry to launch a variety of PEM fuel cell vehicles around the world. Oxygen reduction reaction (ORR) primary research interests include fuel cells and metal-air batteries. The sluggish kinetic reaction of ORR, which is responsible for the rate-limiting reaction at the PEM fuel cell cathodic system, further decreases energy efficiency. Optimising ORR for market expansion with cost-effective and efficient nano-electrocatalysts, on the other hand, remains a challenge. The book covers fundamental ORR reaction kinetics theories, tools, and techniques. It also explains the nano electrocatalysts for ORR made of noble, non-noble, and nanocarbon materials. Finally, the book explores the applications of PEM fuel cells and metal-air batteries.

Photo- and Electro-Catalytic Processes

Photo- and Electro-Catalytic Processes PDF Author: Jianmin Ma
Publisher: John Wiley & Sons
ISBN: 352734859X
Category : Technology & Engineering
Languages : en
Pages : 596

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Book Description
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.

Atomically Precise Metal Nanoclusters

Atomically Precise Metal Nanoclusters PDF Author: Zhikun Wu
Publisher: Morgan & Claypool Publishers
ISBN: 1636390250
Category : Science
Languages : en
Pages : 141

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Book Description
Atomically precise metal nanocluster research has emerged as a new frontier. This book serves as an introduction to metal nanoclusters protected by ligands. The authors have summarized the synthesis principles and methods, the characterization methods and new physicochemical properties, and some potential applications. By pursuing atomic precision, such nanocluster materials provide unprecedented opportunities for establishing precise relationships between the atomic-level structures and the properties. The book should be accessible to senior undergraduate and graduate students, researchers in various fields (e.g., chemistry, physics, materials, biomedicine, and engineering), R&D scientists, and science policy makers.

Direct Methanol Fuel Cells

Direct Methanol Fuel Cells PDF Author: Antonio Salvatore Aricò
Publisher:
ISBN: 9781608768653
Category : Direct energy conversion
Languages : en
Pages : 0

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Book Description
This book deals with an analysis of materials issues, status of technologies and potential applications of direct methanol fuel cells. The principle of operation of direct methanol fuel cells and the status of knowledge in the basic research areas are presented. The technology of direct methanol fuel cells is discussed in this book with particular regard to fabrication methodologies for the manufacturing of catalysts, electrolytes membrane-electrode assemblies, stack hardware and system design.

Nanocarbon Electrochemistry

Nanocarbon Electrochemistry PDF Author: Nianjun Yang
Publisher: John Wiley & Sons
ISBN: 1119468302
Category : Science
Languages : en
Pages : 384

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Book Description
Provides a comprehensive introduction to the field of nanocarbon electrochemistry The discoveries of new carbon materials such as fullerene, graphene, carbon nanotubes, graphene nanoribbon, carbon dots, and graphdiyne have triggered numerous research advances in the field of electrochemistry. This book brings together up-to-date accounts of the recent progress, developments, and achievements in the electrochemistry of different carbon materials, focusing on their unique properties and various applications. Nanocarbon Electrochemistry begins by looking at the studies of heterogeneous electron transfer at various carbon electrodes when redox-active molecules are reversibly and specifically adsorbed on the carbon electrode surface. It then covers electrochemical energy storage applications of various carbon materials, particularly the construction and performance of supercapacitors and batteries by use of graphene and related materials. Next, it concentrates on electrochemical energy conversion applications where electrocatalysis at 0D, 1D, 2D, and 3D carbon materials nanocarbon materials is highlighted. The book finishes with an examination of the contents of electrogenerated chemiluminescence and photoelectrochemical pollutant degradation by use of diamond and related carbon materials. Covers the fundamental properties of different carbon materials and their applications across a wide range of areas Provides sufficient background regarding different applications, which contributes to the understanding of specialists and non-specialists Examines nanoelectrochemistry of adsorption-coupled electron transfer at carbon electrodes; graphene and graphene related materials; diamond electrodes for the electrogenerated chemiluminescence; and more Features contributions from an international team of distinguished researchers Nanocarbon Electrochemistry is an ideal book for students, researchers, and industrial partners working on many diverse fields of electrochemistry, whether they already make frequent use of carbon electrodes in one form of another or are looking at electrodes for new applications.