Issue 3, 2023

Chemistry–mechanics–geometry coupling in positive electrode materials: a scale-bridging perspective for mitigating degradation in lithium-ion batteries through materials design

Abstract

Despite their rapid emergence as the dominant paradigm for electrochemical energy storage, the full promise of lithium-ion batteries is yet to be fully realized, partly because of challenges in adequately resolving common degradation mechanisms. Positive electrodes of Li-ion batteries store ions in interstitial sites based on redox reactions throughout their interior volume. However, variations in the local concentration of inserted Li-ions and inhomogeneous intercalation-induced structural transformations beget substantial stress. Such stress can accumulate and ultimately engender substantial delamination and transgranular/intergranular fracture in typically brittle oxide materials upon continuous electrochemical cycling. This perspective highlights the coupling between electrochemistry, mechanics, and geometry spanning key electrochemical processes: surface reaction, solid-state diffusion, and phase nucleation/transformation in intercalating positive electrodes. In particular, we highlight recent findings on tunable material design parameters that can be used to modulate the kinetics and thermodynamics of intercalation phenomena, spanning the range from atomistic and crystallographic materials design principles (based on alloying, polymorphism, and pre-intercalation) to emergent mesoscale structuring of electrode architectures (through control of crystallite dimensions and geometry, curvature, and external strain). This framework enables intercalation chemistry design principles to be mapped to degradation phenomena based on consideration of mechanics coupling across decades of length scales. Scale-bridging characterization and modeling, along with materials design, holds promise for deciphering mechanistic understanding, modulating multiphysics couplings, and devising actionable strategies to substantially modify intercalation phase diagrams in a manner that unlocks greater useable capacity and enables alleviation of chemo-mechanical degradation mechanisms.

Graphical abstract: Chemistry–mechanics–geometry coupling in positive electrode materials: a scale-bridging perspective for mitigating degradation in lithium-ion batteries through materials design

Article information

Article type
Perspective
Submitted
25 7 2022
Accepted
30 11 2022
First published
08 12 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2023,14, 458-484

Chemistry–mechanics–geometry coupling in positive electrode materials: a scale-bridging perspective for mitigating degradation in lithium-ion batteries through materials design

D. A. Santos, S. Rezaei, D. Zhang, Y. Luo, B. Lin, A. R. Balakrishna, B. Xu and S. Banerjee, Chem. Sci., 2023, 14, 458 DOI: 10.1039/D2SC04157J

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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