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Oriented LiMn₂O₄ Particle Fracture from Delithiation-Driven Surface Stress.

Robert E Warburton¹, Fernando C Castro², Siddharth Deshpande¹

¹Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States.

ACS Applied Materials & Interfaces

|September 25, 2020

Summary

Mechanical fatigue in lithium manganese oxide (LMO) electrodes causes fractures during battery cycling. This study reveals how surface stress during delithiation leads to particle cracking, impacting battery performance.

Keywords:

chemomechanics density functional theory electron microscopy lithiation lithium ion batteries stress

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Published on: July 1, 2013

Area of Science:

Materials Science
Electrochemistry
Computational Chemistry

Background:

Lithium-ion battery electrodes undergo mechanical stress from ion insertion/removal.
Lithium manganese oxide (LMO) electrodes experience surface stress during delithiation, asynchronous with bulk phase transitions.

Purpose of the Study:

To investigate stress evolution and mechanical fracture in LMO electrodes during delithiation.
To understand the chemomechanical response of LMO to electrochemical cycling at a molecular level.

Main Methods:

Integrated approach: cyclic voltammetry, electron microscopy (SEM, TEM, EBSD), and Density Functional Theory (DFT) calculations.
High-rate electrochemical cycling to induce and study mechanical degradation.
DFT modeling of LMO surface mechanical response to delithiation.

Main Results:

Mechanical degradation and fracturing of LMO electrodes were observed, leading to slower kinetics.
DFT calculations indicated tensile stresses near the (001) surface, making fracture unlikely in the [001] direction.
Experimental analysis showed preferential particle fracture along the {111} planes.

Conclusions:

Surface stresses during delithiation contribute significantly to particle fracture in LMO electrodes.
Understanding these chemomechanical processes is crucial for designing robust Li-ion battery materials.