Preface	6
	Contents	8
	1 Atomistic Modeling of Electrode Materials for Li-Ion Batteries: From Bulk to Interfaces	9
	Abstract	9
	1 Introduction	9
	2 Macroscopic Picture of an Electrochemical Reaction	11
	2.1 Microscopic Picture of an Electrochemical Reaction	13
	2.2 Beyond the Thermodynamic Equilibrium	14
	2.3 First-Principles Approach to Condensed Matter	15
	3 Modelization of Bulk Materials	18
	3.1 Equilibrium Crystal Structures	18
	3.2 Finite Temperature Effects	21
	3.3 Electrochemical Properties	24
	4 Modelization of Interfaces	30
	4.1 Surface/Interface Thermodynamics	30
	4.2 First-Principles Approach to Charged Surfaces	33
	4.3 Application to Solid/Liquid Interfaces	35
	4.4 Application to Solid/Solid Interfaces	36
	5 Perspectives	39
	References	40
	2 Multi-scale Simulation Study of Pt-Alloys Degradation for Fuel Cells Applications	45
	Abstract	45
	1 Introduction	45
	2 Time Evolution by Molecular Dynamics and DFT Simulations	48
	3 Time Evolution of PtM Alloys by KMC Methods	51
	4 Degradation of PtCo Skin	57
	5 Concluding Remarks	64
	References	65
	3 Molecular Dynamics Simulations of Electrochemical Energy Storage Devices	68
	Abstract	68
	1 Introduction	69
	2 Molecular Dynamics	71
	2.1 Principle	71
	2.2 All-Atom Force Fields	71
	2.3 Modelling Metallic Electrodes at Constant Potential	72
	2.4 Coarse-Grained Force Fields	73
	3 Li-Ion Batteries	74
	3.1 A Polarizable Force Field Based on First-Principles Calculations	75
	3.2 Conduction Mechanism in Stoichiometric LiMgSO4F	76
	3.3 Effect of Li+ Vacancies	80
	3.4 On the Importance of Finite-Size Effects	82
	4 Supercapacitors	83
	4.1 Increase of the Capacitance in Nanoporous Carbons	83
	4.2 Effect of the Local Structure	86
	4.3 Dynamics of Charging: Coarse-Graining Further	88
	5 Perspectives	89
	References	90
	4 Continuum, Macroscopic Modeling of Polymer-Electrolyte Fuel Cells	97
	Abstract	97
	1 Introduction	97
	1.1 Modeling Dimension	101
	2 Basic Governing Equations	103
	2.1 Material	104
	2.1.1 Charge	106
	2.1.2 Momentum	109
	2.1.3 Energy	110
	3 Membrane	112
	3.1 Membrane Uptake, Morphology, and Function	114
	3.1.1 Calculating Water Uptake	116
	3.2 Transport Equations	119
	3.2.1 General Governing Equations	119
	3.2.2 Choice of Water Driving Force and Transport Parameters	121
	3.2.3 Gas Crossover	123
	3.3 Membrane Swelling	124
	3.4 Contamination and Multi-ion Transport	125
	4 Gas-Diffusion Media	128
	4.1 Modeling Equations	128
	4.1.1 Gas Phase	129
	4.1.2 Liquid Phase	130
	4.1.3 Heat Transport	131
	4.1.4 Liquid/Vapor/Heat Interactions	132
	4.2 Microporous Layers and Pore-Network Modeling	133
	4.3 Transport in the Gas Channel	134
	4.3.1 Droplet Movement	136
	5 Catalyst Layer	137
	5.1 Kinetics	138
	5.2 Transport Phenomena	143
	5.2.1 Agglomerate Length Scale and Ionomer Films	144
	5.3 Electrochemical Impedance Spectroscopy	146
	6 Summary and Future Outlook	149
	References	150
	5 Mathematical Modeling of Aging of Li-Ion Batteries	156
	Abstract	156
	1 Introduction	156
	2 Brief Overview of the Degradation Phenomena in Li-Ion Batteries	160
	2.1 Aging at the Anode	160
	2.2 Aging at the Cathode	163
	3 Mathematical Models	166
	3.1 Performance (Aging-Free) Models	166
	3.1.1 Model of the Elementary Sandwich (``Dualfoil'')	166
	3.1.2 Single-Particle Model	169
	3.2 Modeling of Aging Phenomena	170
	4 Model-Aided Analysis of Battery Aging	177
	4.1 Typical Aging Experiments and Characterization	177
	4.1.1 Aging protocols	177
	4.1.2 Nonintrusive Cell Characterization Techniques	178
	4.1.3 Intrusive Analysis	182
	4.2 ``Snapshot'' Analysis with the Aging-Free Model	185
	4.3 Analysis with the Aging Model	189
	5 Outlook of Physics-Based Aging Modeling	191
	References	192
	6 Fuel Cells and Batteries In Silico Experimentation Through Integrative Multiscale Modeling	196
	Abstract	196
	1 Introduction	197
	1.1 The Role of Computational Electrochemistry	198
	2 Integrative Multiscale Modeling Methods	200
	3 Application Examples	206
	3.1 Microstructurally Resolved Performance Models	206
	3.2 Performance Models with Detailed Electrochemistry	219
	4 Conclusions and Open Challenges	229
	References	233
	7 Cost Modeling and Valuation of Grid-Scale Electrochemical Energy Storage Technologies	239
	Abstract	239
	1 Introduction	240
	2 Methodology	241
	3 Performance Matrix	242
	4 Techno-Economic Cost Modeling	244
	4.1 Analytics Framework	245
	4.2 Determining Storage Benefits	245
	5 Databases	249
	5.1 Database of Storage Technologies	249
	5.2 Database of Storage Applications	250
	6 Storage Valuation	250
	7 Summary and Conclusion	252
	References	252