Atomic-Scale Modelling of Electrochemical Systems (eBook, PDF)

Redaktion: Melander, Marko M.; Laasonen, Kari; Laurila, Tomi T.

• Format: PDF

Produktbeschreibung

Atomic-Scale Modelling of Electrochemical Systems A comprehensive overview of atomistic computational electrochemistry, discussing methods, implementation, and state-of-the-art applications in the field The first book to review state-of-the-art computational and theoretical methods for modelling, understanding, and predicting the properties of electrochemical interfaces. This book presents a detailed description of the current methods, their background, limitations, and use for addressing the electrochemical interface and reactions. It also highlights several applications in electrocatalysis and electrochemistry. Atomic-Scale Modelling of Electrochemical Systems discusses different ways of including the electrode potential in the computational setup and fixed potential calculations within the framework of grand canonical density functional theory. It examines classical and quantum mechanical models for the solid-liquid interface and formation of an electrochemical double-layer using molecular dynamics and/or continuum descriptions. A thermodynamic description of the interface and reactions taking place at the interface as a function of the electrode potential is provided, as are novel ways to describe rates of heterogeneous electron transfer, proton-coupled electron transfer, and other electrocatalytic reactions. The book also covers multiscale modelling, where atomic level information is used for predicting experimental observables to enable direct comparison with experiments, to rationalize experimental results, and to predict the following electrochemical performance. * Uniquely explains how to understand, predict, and optimize the properties and reactivity of electrochemical interfaces starting from the atomic scale * Uses an engaging "tutorial style" presentation, highlighting a solid physicochemical background, computational implementation, and applications for different methods, including merits and limitations * Bridges the gap between experimental electrochemistry and computational atomistic modelling Written by a team of experts within the field of computational electrochemistry and the wider computational condensed matter community, this book serves as an introduction to the subject for readers entering the field of atom-level electrochemical modeling, while also serving as an invaluable reference for advanced practitioners already working in the field.

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Produktdetails

• Verlag: John Wiley & Sons
• Seitenzahl: 368
• Erscheinungstermin: 25. August 2021
• Englisch
• ISBN-13: 9781119605621
• Artikelnr.: 62584890

Autorenporträt

Marko M. Melander, PhD, is a researcher and adjunct professor in physical (electro)chemistry at the University of Jyväskylä in the Department of Chemistry. His work focuses on the development of theory and computational methodologies for studying (proton-coupled) electron transfer thermodynamics and kinetics at electrochemical interfaces. Tomi T. Laurila, PhD is an Associate Professor in the Department of Electrical Engineering and Automation and Department of Chemistry and Materials Science at Aalto University in Finland where he leads the group of Microsystems Technology. The research focus of his group is on electrochemical properties of various carbon nanomaterials, computational materials science and applications of carbon nanomaterials in different sensing devices. Kari Laasonen, PhD, is a Professor in the Department of Chemistry and Materials Science at Aalto University, Finland. He has been working on computational molecular modeling since the early 1990's. He has a strong background in ab initio molecular dynamics and modelling of aqueous systems, and his group started to model electrochemical reactions in early 2010, focusing on hydrogen and oxygen evolution reactions on different catalysts.

Inhaltsangabe

Part I 1

1 Introduction to Atomic Scale Electrochemistry 3
Marko M. Melander, Tomi Laurila, and Kari Laasonen

1.1 Background 3

1.2 The thermodynamics of electrified interface 4

1.2.1 Electrode 6

1.2.2 Electrical double layer 7

1.2.3 Solvation sheets 8

1.2.4 Electrode potential 8

1.3 Chemical interactions between the electrode and redox species 12

1.4 Reaction kinetics at electrochemical interfaces 13

1.4.1 Outer and inner sphere reactions 13

1.4.2 Computational aspects 16

1.4.3 Challenges 17

1.5 Charge transport 18

1.6 Mass transport to the electrode 18

1.7 Summary 19

References 20

Part II 25

2 Retrospective and Prospective Views of Electrochemical Electron Transfer Processes: Theory and Computations 27
Renat R. Nazmutdinov and Jens Ulstrup

2.1 Introduction - interfacial molecular electrochemistry in recent retrospective 27

2.1.1 An electrochemical renaissance 27

2.1.2 A bioelectrochemical renaissance 27

2.2 Analytical theory of molecular electrochemical ET processes 28

2.2.1 A Reference to molecular ET processes in homogeneous solution 28

2.2.2 Brief discussion of contemporary computational approaches 30

2.2.3 Molecular electrochemical ET processes and general chemical rate theory 31

2.2.4 Some electrochemical ET systems at metal electrodes 35

2.2.4.1 Some outer sphere electrochemical ET processes 35

2.2.4.2 Dissociative ET: the electrochemical peroxodisulfate reduction 38

2.2.5 d-band, cation, and spin catalysis 39

2.2.6 New solvent environments in simple electrochemical ET processes - ionic liquids 40

2.2.7 Proton transfer, proton conductivity, and proton coupled electron transfer (PCET) 40

2.2.7.1 Some further notes on the nature of PT/PCET processes 44

2.2.7.2 The electrochemical hydrogen evolution reaction, and the Tafel plot on mercury 44

2.3 Ballistic and stochastic (Kramers-Zusman) chemical rate theory 45

2.4 Early and recent views on chemical and electrochemical long-range ET 50

2.5 Molecular-scale electrochemical science 53

2.5.1 Electrochemical in situ STM and AFM 53

2.5.2 Nanoscale mapping of novel electrochemical surfaces 54

2.5.2.1 Self-assembled molecular monolayers (SAMs) of functionalized thiol [192-194] 54

2.5.3 Electrochemical single-molecule ET and conductivity of complex molecules 56

2.5.4 Selected cases of in situ STM and STS of organic and inorganic redox molecules 58

2.5.4.1 The viologens 58

2.5.4.2 Transition metal complexes as single-molecule in operando STM targets 59

2.5.5 Other single-entity nanoscale electrochemistry 61

2.5.5.1 Electrochemistry in low-dimensional carbon confinement 61

2.5.5.2 Electrochemistry of nano- and molecular-scale metallic nanoparticles 62

2.5.6 Elements of nanoscale and single-molecule bioelectrochemistry 63

2.5.6.1 A single-molecule electrochemical metalloprotein target - P. aeruginosa azurin 63

2.5.6.2 Electrochemical SPMs of metalloenzymes, and some other "puzzles" 65

2.6 Computational approaches to electrochemical surfaces and processes revisited 67

2.6.1 Theoretical methodologies and microscopic structure of electrochemical interfaces 67

2.6.2 The electrochemical process revisited 68

2.7 Quantum and computational electrochemistry in retrospect and prospect 69

2.7.1 Prospective conceptual challenges in quantum and computational electrochemistry 70

2.7.2 Prospec