Electrocatalysis: theoretical foundations and model experiments
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| Other Authors: | |
|---|---|
| Format: | Book |
| Language: | English |
| Published: |
Weinheim
Wiley-VCH
2013
|
| Series: | Advances in electrochemical science and engineering
14 |
| Subjects: | |
| Online Access: | Inhaltsverzeichnis Klappentext |
| Physical Description: | XVI, 303 S. Ill., graph. Darst. |
| ISBN: | 9783527332274 9783527680436 |
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| 245 | 1 | 0 | |a Electrocatalysis |b theoretical foundations and model experiments |c ed. by Richard C. Alkire ... |
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| 300 | |a XVI, 303 S. |b Ill., graph. Darst. | ||
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| adam_text | VII
Contents
ρ
Preface
XIII
List of Contributors XV
Ί
Muniscale
Modeling of Electrochemical Systems
1
Jonathan E. Mueller,
Donato
Fantauzzi, and
Timo
Jacob
1.1
Introduction I
1.2
Introduction to Multiscale Modeling
3
1.3
Electronic Structure Modeling
6
1.3.1
Modern Electronic Structure Theory
6
1.3.1.1
Quantum Mechanical Foundations
6
1.3.1.2
Born—
Oppenheimer
Approximation
8
1.3.1.3
Single-Electron Hamiltonians
9
1.3.1.4
Basis Sets
10
1.3.1.5
Enforcing the
Pauli
Principle
11
1.3.1.6
Electron Correlation Methods
12
1.3.1.7
Density Functional Theory
14
1.3.2
Applications of Electronic Structure to Geometric Properties
16
1.3.2.1
Geometry Optimization
16
1.3.2.2
Transition State Searches
17
1.3.3
Corrections to Potential Energy Surfaces and Reaction Pathways
18
1.3.3.1
Energy and Entropy Corrections
18
1.3.3.2
Thermodynamic State Functions
20
1.3.3.3
Reaction Energies and Rates
21
1.3.4
Electronic Structure Models in Electrochemistry
22
1.3.4.1
Modeling the Electrode Surface: Cluster versus Slab
23
1.3.4.2
Modeling the Solvent: Explicit versus Implicit
24
1.3.4.3
Modeling the Electrode Potential
25
1.3.5
Summary
26
1.4
Molecular Simulations
27
1.4.1
Energy Terms and Force Field Parameters
27
1.4.1.1
Covalent Bond Interactions
27
1.4.1.2
Non-Covalent Interactions
32
1.4.2
Parametrization and Validation
34
1.4.3
Atomistic Simulations
35
Vlil I
Contents
1.4.3.1
Monte Carlo Methods
35
1.4.3.2
Molecular Dynamics
36
1.4.3.3
QM/MM
37
1.4.4
Sampling and Analysis
3 9
1.4.5
Applications of Molecular Modeling in Electrochemistry
39
1.4.6
Summary
40
1.5
Reaction Modeling
40
1.5.1
Introduction
40
1.5.2
Chemical Kinetics
41
1.5.3
Kinetic Monte Carlo
41
1.5.3.1
System States and the Lattice Approximation
41
1.5.3.2
Reaction Rates
42
1.5.3.3
Reaction Dynamics
43
1.5.3.4
Applications of
кМС
in Electrochemistry
45
1.5.4
Summary
45
1.6
The Oxygen Reduction Reaction on Pt(l
11) 46
1.6.1
Introduction to the Oxygen Reduction Reaction
46
1.6.2
Preliminary Considerations
46
1.6.3
DFT Calculations
48
1.6.4
Method Validation
49
1.6.5
Reaction Energies
49
1.6.6
Solvation Effects
51
1.6.7
Free Energy Contributions
52
1.6.8
Influence of an Electrode Potential
53
1.6.9
Modeling the Kinetic Rates
55
1.6.10
Summary
58
1.7
Formic Acid Oxidation on Pt(l
11 ) 59
1.7.1
Introduction to Formic Acid Oxidation
59
1.7.2
Density Functional Theory Calculations
60
1.7.3
Gas Phase Reactions
60
1.7.4
Explicit Solvation Model
61
1.7.5
Eley—Rideal Mechanisms and the Electrode Potential
63
1.7.6
Kinetic Rate Model of Formic Acid Oxidation
65
1.7.7
Summary
66
1.8
Concluding Remarks
66
References
67
2
Statistical Mechanics and Kinetic Modeling of Electrochemical Reactions
on Single-Crystal Electrodes Using the Lattice-Gas Approximation
75
Marc
T.M. Koper
2.1
Introduction
75
2.2
Lattice-Gas Modeling of Electrochemical Surface Reactions
76
2.3
Statistical Mechanics and Approximations
79
2.3.1
Static System
79
2.3.2
Dynamical System
83
Contents
І
IX
2.4 Monte Carlo
Simulations
84
2.5 Applications
to
Electrosorption, Electrodeposition and
Electrocatalysis 85
2.5.1 Electrosorption and Electrodeposition 85
2.5.2 Electrocatalysis 92
2.6
Conclusions
96
References
96
3 Single
Molecular Electrochemistry within an STM
99
RichardJ. Nichols and Simon J. Higgins
З.Д
Introduction
99
3.2
Experimental Methods for Single Molecule Electrical Measurements
in Electrochemical Environments
101
3.3
Electron Transfer Mechanisms
103
3.3.1
Tunneling
106
3.3.2
Resonant Tunneling
109
3.3.3
Hopping Models 111
3.4
Single Molecule Electrochemical Studies with an STM
115
3.4.1
Adsorbed Iron Complexes
115
3.4.2
Viologens
118
3.4.3
Osmium and Cobalt Metal Complexes
122
3.4.4
PyrroloTTF (pTTF)
125
3.4.5
Perylene Tetracarboxylic Diimides
128
3.4.6
Oligo(phenylene ethynylene)
Derivates 130
3.5
Conclusions and Outlook
131
References
134
4
From Microbial Bioelectrocatalysis to Microbial Bioelectroc
nemicai
Systems
137
Uwe Schröder
and
Falk
Harnisch
4.1
Prelude: From Fundamentals to Biotechnology
137
4.2
Microbial BioelectrochemicaJ Systems (BESs)
137
4.2
Л
The Archetype: Microbial Fuel Cells (MFCs)
137
4.2.2
Strength Through Diversity: Microbial Bioelectrochemical
Systems
139
4.3
Bioelectrocatalysis: Microorganisms Catalyze Electrochemical
Reactions
140
4.3.1
Energetic Considerations of Microbial Bioelectrocatalysis
141
4.3.1.1
Case Study: The Anodic Acetate Oxidation by Geobacteraceae
142
4.3.1.2
Case Study: The Cathodic Hydrogen Evolution Reaction (HER)
143
4.3.2
Microbial Electron Transfer Mechanisms
144
4.3.2.1
Direct Electron Transfer
(DET)
244
4.3.2.2
Mediated Electron Transfer (MET)
146
4.3.2.3
Cathodic Electron Transfer Mechanisms
148
4.3.3
Microbial Interactions: Ecological Networks
148
Χ Ι
Contents
4.3.3.1
Interspecies
Electron Transfer and Scavenging of
Redox-
Shuttles
148
4.4
Characterizing Anodic
Biofilms
by Electrochemical and Biological
Means
249
4.4.1.1
Case Study: On the use of Cyclic Voltammetry
154
4.4.1.2
Case Study: Raman Microscopy
155
References
156
5
Electrocapillarity of Solids and its Impact on Heterogeneous
Catalysis
163
Jörg
Weissm ùller
5.1
Introduction
163
5.2
Mechanics of Solid Electrodes
164
5.2.1
Outline
-
Surface Stress and Surface Tension
164
5.2.2
Solid Versus Fluid
167
5.2.3
Free Energy of Elastic Solid Surfaces
267
5.2.4
Deforming a Solid Surface
270
5.2.5
Case Study: Thought Experiment in Electrowetting
2 72
5.2.6
Capillary Equations for Fluids and Solids
275
5.2.7
Case Study: Molecular Dynamics Study of Surface-Induced
Pressure
277
5.3
Electrocapillary Coupling at Equilibrium
177
5.3.1
Outline
—
Polarizable and Nonpolarizable Electrodes
277
5.3.2 Lippmann
Equation and Electrocapillary Coupling Coefficient
279
5.3.3
Case Study: Cantilever-Bending Experiment in Electrolyte
282
5.3.4
Important Maxwell Relations for Electrocapillarity
183
5.3.5
Electrocapillary Coupling During Electrosorption
284
5.3.6
Coupling Coefficient for Adsorption from Gas
185
5.3.7
Coupling Coefficient for the Langmuir Isotherm
286
5.3.8
Case Study: Strain-Dependent Hydrogen
Underpotential
Deposition
187
5.3.9
Coupling Coefficient for Potential of Zero Charge and Work
Function
290
5.3.10
Empirical Data for the Electrocapillary Coupling Coefficient
293
5.4
Exploring the Dynamics
298
5.4.1
Outline
298
5.4.2
Cyclic Cantilever-Bending Experiments
299
5.4.3
Dynamic Electro-Chemo-Mechanical Analysis
200
5.5
Mechanically Modulated Catalysis
203
5.5.1
Outline
203
5.5.2
Phenomenology: Distinguishing
Capacitive
from Faraday Current
204
5.5.3
Rate equations:
Butler-Volmer
kinetics
206
5.5.4
Rate Equations: Heyrowsky Reaction
207
5.6
Summary and Outlook
222
References
225
Contents
І
XI
6
Synthesis of Precious Metal Nanoparticles with High Surface
Energy and High Electrocatalytic Activity
221
Long Huang, Zhi-You Zhou,
Na Tian,
and Shi-Gang Sun
6.1
Introduction
221
6.2
Shape-Controlled Synthesis of Monometallic Nanocrystals
with High Surface Energy
224
6.2.1
Electrochemical Route
224
6.2.1.1
Platinum
224
6.2.1.2
Palladium
228
6.2.2
Wet-Chemical Route
230
6.2.2.1
Platinum
230
6.2.2.2
Palladium
232
6.2.2.3
Gold
234
6.3
Shape-Controlled Synthesis of Bimetallic NCs with
High Surface Energy
235
6.3.1
Surface Modification
236
6.3.1.1
Bi-ModifiedTHHPtNCs
237
6.3.1.2
Ru-ModifiedTHH PtNCs
239
6.3.1.3
Au-ModrfiedPtTHHNCs
241
6.3.1.4
Pt-Modified
Au
Prisms with High-Index Facets
243
6.3.2
Alloy NCs
245
6.3.2.1
THHPdPt Alloy
245
6.3.2.2
НОН
PdAu Alloy
247
6.3.3
Core-Shell Structured NCs
248
6.4
Concluding Remarks and Perspective
254
References
256
7
Х
-Ray Studies of Strained Catalytic Dealloyed Pt Surfaces
259
Peter Strasser
7.1
Introduction
259
7.2
Dealloyed Bimetallic Surfaces
262
7.3
Dealloyed Strained Pt Core-Shell Model Surfaces
264
7.4
Х
-Ray Studies of Dealloyed Strained PtCu3(lll) Single Crystal
Surfaces
266
7.5
Х
-Ray Studies of Dealloyed Strained Pt-Cu Polycrystalline
Thin Film Surfaces
269
7.6
Х
-Ray Studies of Dealloyed Strained Alloy
Nanoparticles
273
7.6.1
Bragg
Brentano
Powder
Х
-Ray Diffraction (XRD)
273
7.6.2
In Situ High Temperature Powder
Х
-Ray Diffraction
(XRD)
274
7.6.3
Synchrotron
Х
-Ray
Photoemission
Spectroscopy (XPS)
276
7.6.4
Anomalous Small Angle
Х
-Ray Scattering (ASAXS)
277
7.6.5
Anomalous Powder
Х
-Ray Diffraction (AXRD)
277
XII
I Contents
7.6.6
High Energy
Х
-Ray Diffraction (HE-XRD) and Atomic Pair
Distribution Function (PDF) Analysis
287
7.7
Conclusions
284
References
285
Index
293
Advances in Electrochemical Science and Engineering
Volume
14
Electrocatalysis
Catalysts speed up a chemical reaction or allow for reactions to take
place that would not otherwise occur. The chemical nature of a catalyst
and its structure are crucial for interactions with reaction intermediates.
An electrocatalyst is used in an electrochemical reaction, for example
in a fuel cell to produce electricity. In this case, reaction rates are also
dependent on the electrode potential and the structure of the electrical
double-layer.
This work provides a valuable overview of this rapidly developing
field by focusing on the aspects that drive the research of today and to¬
morrow. Key topics are discussed by leading experts, making this book a
must-have for many scientists of the field with backgrounds in different
disciplines, including chemistry, physics, biochemistry, engineering as
well as surface and materials science. This book is volume
XIV
in the
series Advances in Electrochemical Sciences and Engineering*.
The editors:
Richard
С
Aliare,
Department of Chemical Engineering,
University of Illinois,
Urbana, USA
Ludwig
A. Kibier, Institute of Electrochemistry,
University of
Ulm,
Germany
Dicier M.
Kolb,
Institute of Electrochemistry,
University of
Ulm,
Germany
Jacek Lipkowski,
Department of Chemistry,
University of Guelph, Canada
|
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| dewey-ones | 572 - Biochemistry |
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| discipline | Chemie / Pharmazie Physik Biologie Chemie |
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| indexdate | 2024-07-10T00:57:38Z |
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| series | Advances in electrochemical science and engineering |
| series2 | Advances in electrochemical science and engineering |
| spelling | Electrocatalysis theoretical foundations and model experiments ed. by Richard C. Alkire ... Weinheim Wiley-VCH 2013 XVI, 303 S. Ill., graph. Darst. txt rdacontent n rdamedia nc rdacarrier Advances in electrochemical science and engineering 14 Elektrokatalyse (DE-588)4151819-6 gnd rswk-swf (DE-588)4143413-4 Aufsatzsammlung gnd-content Elektrokatalyse (DE-588)4151819-6 s DE-604 Alkire, Richard C. 1941- (DE-588)136277446 edt Erscheint auch als Online-Ausgabe, EPUB 978-3-527-68045-0 Erscheint auch als Online-Ausgabe, MOBI 978-3-527-68044-3 Erscheint auch als Online-Ausgabe, PDF 978-3-527-68046-7 Advances in electrochemical science and engineering 14 (DE-604)BV004176465 14 Digitalisierung UB Bayreuth - ADAM Catalogue Enrichment application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=026922066&sequence=000003&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis Digitalisierung UB Bayreuth - ADAM Catalogue Enrichment application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=026922066&sequence=000004&line_number=0002&func_code=DB_RECORDS&service_type=MEDIA Klappentext |
| spellingShingle | Electrocatalysis theoretical foundations and model experiments Advances in electrochemical science and engineering Elektrokatalyse (DE-588)4151819-6 gnd |
| subject_GND | (DE-588)4151819-6 (DE-588)4143413-4 |
| title | Electrocatalysis theoretical foundations and model experiments |
| title_auth | Electrocatalysis theoretical foundations and model experiments |
| title_exact_search | Electrocatalysis theoretical foundations and model experiments |
| title_full | Electrocatalysis theoretical foundations and model experiments ed. by Richard C. Alkire ... |
| title_fullStr | Electrocatalysis theoretical foundations and model experiments ed. by Richard C. Alkire ... |
| title_full_unstemmed | Electrocatalysis theoretical foundations and model experiments ed. by Richard C. Alkire ... |
| title_short | Electrocatalysis |
| title_sort | electrocatalysis theoretical foundations and model experiments |
| title_sub | theoretical foundations and model experiments |
| topic | Elektrokatalyse (DE-588)4151819-6 gnd |
| topic_facet | Elektrokatalyse Aufsatzsammlung |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=026922066&sequence=000003&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=026922066&sequence=000004&line_number=0002&func_code=DB_RECORDS&service_type=MEDIA |
| volume_link | (DE-604)BV004176465 |
| work_keys_str_mv | AT alkirerichardc electrocatalysistheoreticalfoundationsandmodelexperiments |