An efficient approach to include transport effects in thin coating layers in electrochemo-mechanical models for all-solid-state batteries

A novel approach is presented to efficiently include transport effects in thin active material coating layers of all-solid-state batteries using a dimensionally reduced formulation embedded into a three-dimensionally resolved coupled electrochemo-mechanical continuum model. In the literature, the effect of coating layers is so far captured by additional zero-dimensional resistances to circumvent the need for an extremely fine mesh resolution. However, a zero-dimensional resistance cannot capture transport phenomena along the coating layer, which can become significant, as we will show in this work. Thus, we propose a model which resolves the thin coating layer in a two-dimensional manifold based on model assumptions in the direction of the thickness. This two-dimensional formulation is monolithically coupled with a three-dimensional model representing the other components of a battery cell. The approach is validated by showing conservation properties and convergence and by comparing the results with those computed with a fully resolved model. Results for realistic microstructures of a battery cell, including coating layers as well as design recommendations for a preferred coating layer, are presented. Based on those results, we show that existing modeling approaches feature remarkable errors when transport along the coating layer is significant, whereas the novel approach resolves this.

[1]  J. Janek,et al.  Challenges in speeding up solid-state battery development , 2023, Nature Energy.

[2]  Xiang Chen,et al.  Review on the lithium transport mechanism in solid‐state battery materials , 2022, WIREs Computational Molecular Science.

[3]  B. Gates,et al.  Review—Surface Coatings for Cathodes in Lithium Ion Batteries: From Crystal Structures to Electrochemical Performance , 2022, Journal of The Electrochemical Society.

[4]  T. Brezesinski,et al.  Advanced Nanoparticle Coatings for Stabilizing Layered Ni‐Rich Oxide Cathodes in Solid‐State Batteries , 2022, Advanced Functional Materials.

[5]  S. Choudhury,et al.  Effects of Polymer Coating Mechanics at Solid‐Electrolyte Interphase for Stabilizing Lithium Metal Anodes , 2021, Advanced Energy Materials.

[6]  J. Sann,et al.  Analyzing Nanometer-Thin Cathode Particle Coatings for Lithium-Ion Batteries—The Example of TiO2 on NCM622 , 2021, ACS Applied Energy Materials.

[7]  Sehee Lee,et al.  Effect of Amorphous LiPON Coating on Electrochemical Performance of LiNi0.8Mn0.1Co0.1O2 (NMC811) in All Solid-State Batteries , 2021 .

[8]  I. Belharouak,et al.  Valuation of Surface Coatings in High-Energy Density Lithium-ion Battery Cathode Materials , 2021 .

[9]  J. Sann,et al.  The Working Principle of a Li2CO3/LiNbO3 Coating on NCM for Thiophosphate-Based All-Solid-State Batteries , 2021 .

[10]  Felix H. Richter,et al.  Analysis of Interfacial Effects in All-Solid-State Batteries with Thiophosphate Solid Electrolytes. , 2020, ACS applied materials & interfaces.

[11]  M. Wohlfahrt‐Mehrens,et al.  Manufacturing Process for Improved Ultra‐Thick Cathodes in High‐Energy Lithium‐Ion Batteries , 2020, Energy Technology.

[12]  M. Koyama,et al.  Multi-Physics Simulation of Solid-State Batteries with Active Material Coating , 2020 .

[13]  Christian Masquelier,et al.  Fundamentals of inorganic solid-state electrolytes for batteries , 2019, Nature Materials.

[14]  M. Kronbichler,et al.  Parallel, physics-oriented, monolithic solvers for three-dimensional, coupled finite element models of lithium-ion cells , 2019, Computer Methods in Applied Mechanics and Engineering.

[15]  J. Janek,et al.  On the Functionality of Coatings for Cathode Active Materials in Thiophosphate‐Based All‐Solid‐State Batteries , 2019, Advanced Energy Materials.

[16]  J. Janek,et al.  Chemo-mechanical expansion of lithium electrode materials – on the route to mechanically optimized all-solid-state batteries , 2018 .

[17]  W. Wall,et al.  A monolithic, mortar‐based interface coupling and solution scheme for finite element simulations of lithium‐ion cells , 2018 .

[18]  S. Dou,et al.  Novel surface coating strategies for better battery materials , 2017 .

[19]  K. Zhao,et al.  Electronic Structure and Comparative Properties of LiNixMnyCozO2 Cathode Materials , 2017 .

[20]  W A Wall,et al.  A biochemo-mechano coupled, computational model combining membrane transport and pericellular proteolysis in tissue mechanics , 2017, Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences.

[21]  Jürgen Janek,et al.  A solid future for battery development , 2016, Nature Energy.

[22]  Joon-Hyung Lee,et al.  Mixed Electronic and Ionic Conductor-Coated Cathode Material for High-Voltage Lithium Ion Battery. , 2016, ACS applied materials & interfaces.

[23]  Wolfgang A. Wall,et al.  Unified computational framework for the efficient solution of n-field coupled problems with monolithic schemes , 2016, 1605.01522.

[24]  Z. Wen,et al.  Electronic and ionic co-conductive coating on the separator towards high-performance lithium–sulfur batteries , 2016 .

[25]  D. Morgan,et al.  Lithium transport through lithium-ion battery cathode coatings , 2015, 1607.02125.

[26]  Qinglin Wang,et al.  Mixed conduction and grain boundary effect in lithium niobate under high pressure , 2015 .

[27]  Jianping Long,et al.  First-principles investigations of the physical properties of lithium niobate and lithium tantalate , 2013 .

[28]  C. Wolverton,et al.  Lithium Transport in Amorphous Al2O3 and AlF3 for Discovery of Battery Coatings , 2013 .

[29]  Kazunori Takada,et al.  Progress and prospective of solid-state lithium batteries , 2013 .

[30]  Petros Koumoutsakos,et al.  Simulations of (an)isotropic diffusion on curved biological surfaces. , 2006, Biophysical journal.

[31]  Phillip Colella,et al.  Numerical computation of diffusion on a surface. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[32]  K. Nassau,et al.  Ionic conductivity of quenched alkali niobate and tantalate glasses , 1978 .

[33]  L. Giordano,et al.  Coating-Dependent Electrode-Electrolyte Interface for Ni-Rich Positive Electrodes in Li-Ion Batteries , 2019 .

[34]  K. Zhao,et al.  Electronic Structure and Comparative Properties of LiNi x Mn y Co z O 2 Cathode Materials , 2017 .

[35]  K. Zhao,et al.  Mechanical and Structural Degradation of LiNixMnyCozO2 Cathode in Li-Ion Batteries: An Experimental Study , 2017 .

[36]  Eric P. Holowka,et al.  Thin-Film Materials , 2014 .

[37]  A. Ibrahimbegovic Nonlinear Solid Mechanics , 2009 .

[38]  S. Rosenberg The Laplacian on a Riemannian Manifold: The Laplacian on a Riemannian Manifold , 1997 .