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On the Fundamental and Practical Aspects of Modeling Complex Electrochemical Kinetics and Transport

Journal Article · · Journal of the Electrochemical Society
DOI:https://doi.org/10.1149/2.0241813jes· OSTI ID:1475263
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Numerous technologies, such as batteries and fuel cells, depend on electrochemical kinetics. In some cases, the responsible electrochemistry and charged-species transport is complex. However, to date, there are essentially no general-purpose modeling capabilities that facilitate the incorporation of thermodynamic, kinetic, and transport complexities into the simulation of electrochemical processes. A vast majority of the modeling literature uses only a few (often only one) global charge-transfer reactions, with the rates expressed using Butler-Volmer approximations. The objective of the present paper is to identify common aspects of electrochemistry, seeking a foundational basis for designing and implementing software with general applicability across a wide range of materials sets and applications. The development of new technologies should be accelerated and improved by enabling the incorporation of electrochemical complexity (e.g., multi-step, elementary charge-transfer reactions and as well as supporting ionic and electronic transport) into the analysis and interpretation of scientific results. The spirit of the approach is analogous to the role that Chemkin has played in homogeneous chemistry modeling, especially combustion. The Cantera software, which already has some electrochemistry capabilities, forms the foundation for future capabilities expansion.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); U.S. Air Force Office of Scientific Research; US Department of the Navy, Office of Naval Research (ONR)
DOE Contract Number:
AC36-08GO28308
OSTI ID:
1475263
Report Number(s):
NREL/JA-5400-71849
Journal Information:
Journal of the Electrochemical Society, Vol. 165, Issue 13; ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English

References (77)

Modeling detailed chemistry and transport for solid-electrolyte-interface (SEI) films in Li–ion batteries December 2011
Theories and Problems of Liquid Diffusion November 1945
Experimental determination of the Onsager coefficients of transport for Ce0.8Pr0.2O2−δ January 2010
Diffuse-charge dynamics in electrochemical systems August 2004
Defect-Transport-Induced Stress in Mixed Ionic-Electronic Conducting (MIEC) Ceramic Membranes January 2016
Impact of Li 2 O 2 Particle Size on Li–O 2 Battery Charge Process: Insights from a Multiscale Modeling Perspective September 2016
Membrane polarization in mixed-conducting ceramic fuel cells and electrolyzers January 2016
Simulation and Optimization of the Dual Lithium Ion Insertion Cell January 1994
Analytical Theories of Transport in Concentrated Electrolyte Solutions from the MSA May 2005
Equilibrium and transient conductivity for gadolinium-doped ceria under large perturbations: I. Experiments November 2014
Equilibrium and transient conductivity for gadolium-doped ceria under large perturbations: II. Modeling December 2014
Readily processed protonic ceramic fuel cells with high performance at low temperatures July 2015
Electron-Ion Interference and Onsager Reciprocity in Mixed Ionic-Electronic Transport in TiO 2 December 2006
Resolving a Discrepancy in Diffusion Potentials, with a Case Study for Li-Ion Batteries January 2016
Process intensification in the catalytic conversion of natural gas to fuels and chemicals January 2017
In Situ and Quantitative Characterization of Solid Electrolyte Interphases February 2014
Effective potential theory for diffusion in binary ionic mixtures January 2017
Impact of non-ideal behavior on ignition delay and chemical kinetics in high-pressure shock tube reactors March 2018
Thermodynamically consistent modeling of elementary electrochemistry in lithium-ion batteries December 2010
Battery materials for ultrafast charging and discharging March 2009
Modeling Protonic-Ceramic Fuel Cells with Porous Composite Electrodes in a Button-Cell Configuration January 2017
Mechanistic modeling of polysulfide shuttle and capacity loss in lithium–sulfur batteries August 2014
A Critical Review of the Li Insertion Mechanisms in LiFePO 4 Electrodes January 2013
Modeling Electrochemical Oxidation of Hydrogen on Ni–YSZ Pattern Anodes January 2009
The effect of hydrogen crossover on open-circuit voltage in polymer electrolyte membrane fuel cells April 2010
Solid Electrolyte Interphase in Li-Ion Batteries: Evolving Structures Measured In situ by Neutron Reflectometry May 2012
Multistep Reaction Mechanisms in Nonaqueous Lithium–Oxygen Batteries with Redox Mediator: A Model-Based Study October 2016
Interpretation of Defect and Gas-Phase Fluxes through Mixed-Conducting Ceramics Using Nernst–Planck–Poisson and Integral Formulations October 2013
Computational modeling of sodium-iodine secondary batteries November 2016
Nonequilibrium Thermodynamics of Porous Electrodes January 2012
Thermo-electrochemical production of compressed hydrogen from methane with near-zero energy loss November 2017
Defect structure and defect-induced expansion of doped perovskite La 0.7 Sr 0.3 Co 0.9 Fe 0.1 O 3−δ December 2014
Chemical Expansion: Implications for Electrochemical Energy Storage and Conversion Devices July 2014
Electrode Materials for Rechargeable Sodium-Ion Batteries: Potential Alternatives to Current Lithium-Ion Batteries May 2012
Understanding chemical expansion in perovskite-structured oxides January 2015
Irreversible Processes in Electrolytes. Diffusion, Conductance and Viscous Flow in Arbitrary Mixtures of Strong Electrolytes November 1932
Relaxation Phenomena in Lithium-Ion-Insertion Cells January 1994
Full-Range Simulation of a Commercial LiFePO 4 Electrode Accounting for Bulk and Surface Effects: A Comparative Analysis December 2013
Highly durable, coking and sulfur tolerant, fuel-flexible protonic ceramic fuel cells May 2018
Mathematical modeling of porous battery electrodes—Revisit of Newman's model April 2011
Transport Equations for a Mixture of Two Binary Molten Salts in a Porous Electrode January 1979
Multimodal Physics-Based Aging Model for Life Prediction of Li-Ion Batteries January 2009
Single-Particle Model for a Lithium-Ion Cell: Thermal Behavior January 2011
Modeling of Galvanostatic Charge and Discharge of the Lithium/Polymer/Insertion Cell January 1993
Influence of local lithium metal deposition in 3D microstructures on local and global behavior of Lithium-ion batteries May 2016
Electrodes with High Power and High Capacity for Rechargeable Lithium Batteries February 2006
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation July 2013
Effects of three-dimensional cathode microstructure on the performance of lithium-ion battery cathodes January 2013
Comment on “How to interpret Onsager cross terms in mixed ionic electronic conductors” by I. Riess, Phys. Chem. Chem. Phys., 2014, 16 , 22513 January 2015
Theory of Onsager phenomenological coefficients for isothermal linear transport processes in electrolyte solutions August 1984
Direct conversion of methane to aromatics in a catalytic co-ionic membrane reactor August 2016
Mass Transfer in Concentrated Binary Electrolytes September 1965
Modeling Distributed Charge-Transfer Processes in SOFC Membrane Electrode Assemblies January 2008
On the correlation between surface chemistry and performance of graphite negative electrodes for Li ion batteries September 1999
Building better batteries February 2008
Mesoscopic Modeling of a LiFePO 4 Electrode: Experimental Validation under Continuous and Intermittent Operating Conditions January 2017
Interaction between diffusion and chemical stresses November 2005
The thermodynamic origin of hysteresis in insertion batteries April 2010
Particle-Level Modeling of the Charge-Discharge Behavior of Nanoparticulate Phase-Separating Li-Ion Battery Electrodes January 2014
Modeling Elementary Heterogeneous Chemistry and Electrochemistry in Solid-Oxide Fuel Cells January 2005
Concentration-Dependent Chemical Expansion in Lithium-Ion Battery Cathode Particles June 2014
A Mathematical Model for the Lithium-Ion Negative Electrode Solid Electrolyte Interphase January 2004
Progress in the direct catalytic conversion of methane to fuels and chemicals July 2016
Physical chemistry of some microstructural phenomena October 1978
Chemical Expansivity of Electrochemical Ceramics September 2001
Assessing Electrolyte Transport Properties with Molecular Dynamics January 2017
Theory of Chemical Kinetics and Charge Transfer based on Nonequilibrium Thermodynamics June 2012
Asymmetry of Discharge/Charge Curves of Lithium-Ion Battery Intercalation Electrodes October 2016
A Flexible Framework for Modeling Multiple Solid, Liquid and Gaseous Phases in Batteries and Fuel Cells January 2012
A promising cathode for intermediate temperature protonic ceramic fuel cells: BaCo0.4Fe0.4Zr0.2O3−δ January 2013
Multi-Scale Thermo-Electrochemical Modeling of Performance and Aging of a LiFePO 4 /Graphite Lithium-Ion Cell December 2016
Zr and Y co-doped perovskite as a stable, high performance cathode for solid oxide fuel cells operating below 500 °C January 2017
Catalytic Chemistry for Methane Dehydroaromatization (MDA) on a Bifunctional Mo/HZSM-5 Catalyst in a Packed Bed September 2016
Interpreting equilibrium-conductivity and conductivity-relaxation measurements to establish thermodynamic and transport properties for multiple charged defect conducting ceramics January 2015
The influence of equilibrium potential on the hydrogen oxidation kinetics of SOFC anodes January 2007
Precipitation in aqueous lithium–oxygen batteries: a model-based analysis January 2013
Discharge Model for the Lithium Iron-Phosphate Electrode January 2004

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