3D Heterogeneous Model for Electrodes in Lithium-Ion Batteries to Study Interfacial Detachment of Active Material Particles and Carbon-Binder Domain

Author:

Mirsalehian Mohammadali1,Vossoughi Bahareh1,Kaiser Jörg2,Pischinger Stefan12

Affiliation:

1. Chair of Thermodynamics of Mobile Energy Conversion Systems (TME), RWTH Aachen University, Forckenbeckstraße 4, 52074 Aachen, Germany

2. FEV Europe GmbH, Neuenhofstraße 181, 52078 Aachen, Germany

Abstract

Mechanics plays a crucial role in the performance and lifespan of lithium-ion battery (LIB) cells. Thus, it is important to address the interplay between electrochemistry and mechanics in LIBs, especially when aiming to enhance the energy density of electrodes. Accordingly, this work introduces a framework for a fully coupled electro-chemo-mechanical heterogeneous 3D model that allows resolving the inhomogeneities accompanied by electrochemical and mechanical responses of LIB electrodes during operation. The model is employed to numerically study the mechanical degradation of a nickel manganese cobalt (NMC) cathode electrode, assembled in a half-cell, upon cycling. As opposed to previous works, a virtual morphology for a high-energy electrode with low porosity is developed in this study, which comprises distinct domains of active material (AM) particles, the carbon-binder domain (CBD), and the pore domain to resemble real commercial electrodes. It is observed that the mechanical strain mismatch between irregularly and randomly positioned AM particles and the CBD might lead to local contact detachment. This interfacial gap, in combination with the diminishing contact strength over cell cycling, continuously deteriorates the electrode performance upon cycling by impedance rise and capacity drop. In agreement with previous experimental reports, the presented simulation results exhibit that the contact loss mostly takes place in the regions closer to the separator. Eventually, the resulting gradual capacity drop and change in impedance spectrum over cycling, as the consequence of interfacial gap formation, are discussed and indicated.

Publisher

MDPI AG

Subject

Energy (miscellaneous),Energy Engineering and Power Technology,Renewable Energy, Sustainability and the Environment,Electrical and Electronic Engineering,Control and Optimization,Engineering (miscellaneous),Building and Construction

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