Decoupling the effects of surface morphology and interfacial chemistry on localized electrochemical kinetics in LiCoO2 cathodes
6 affiliations
- 1School of Chemistry, Xi'an Jiaotong University Xi'an 710049 China
- 2School of Future Technology, Xi'an Jiaotong University Xi'an 710049 China
- 3Xi'an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences Xi'an 710119 China
- 4Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi'an Jiaotong University Xi'an 710049 China
- 5Instrumental Analysis Center of Xi'an Jiaotong University Xi'an 710049 China
- 6Ningxia Advanced Intelligent Sensing and Control Technology Innovation Team, Ningxia Key Laboratory of Bioimaging and Intelligent Diagnostics, North Minzu University Yinchuan 750021 China
Abstract
Spatial heterogeneity at electrode/electrolyte interfaces critically influences the electrochemical performance and degradation of lithium-ion batteries, yet the respective contributions of surface morphology and interfacial chemistry to localized electrochemical kinetics remain difficult to distinguish experimentally. Existing characterization techniques reveal either material structural transformation or chemical reconstruction but cannot quantitatively decouple their individual effects on local electrochemical behaviour. Herein, we establish a correlative multimodal strategy by integrating scanning electrochemical cell microscopy (SECCM), atomic force microscopy (AFM), Raman spectroscopy, and finite-element modelling to investigate the spatiotemporal evolution of LiCoO2 thin films during environmental exposure. Spatially resolved SECCM measurements reveal distinct microdomain-dependent electrochemical heterogeneity despite the initially homogeneous structure of the films. Correlative structural and chemical analyses, together with quantitative simulations, demonstrate that surface morphology and interfacial chemistry govern distinct aspects of the electrochemical response. By independently introducing the roughness factor and the effective lithium-ion diffusion coefficient into the multiphysics model, these two contributions can be quantitatively decoupled, with morphology predominantly determining the current response amplitude and interfacial chemistry governing kinetic limitations. This work provides a distinct strategy for correlating local interfacial evolution with electrochemical function and offers new insights into heterogeneous electrochemical interfaces in advanced energy-storage materials.
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BibTeX
@article{guan2026decoupling,
title = {{Decoupling the effects of surface morphology and interfacial chemistry on localized electrochemical kinetics in LiCoO2 cathodes}},
author = {Yuxia Guan and Pingshi Wang and Ning Gao and Penghui Liu and Weiwei Cao and Shujiang Ding and Lingjie Meng and Kai Xi and Rui Gao},
journal = {Chemical Science},
year = {2026},
month = sep,
doi = {10.1039/d6sc06380b},
url = {https://doi.org/10.1039/d6sc06380b},
note = {CC BY 3.0},
}
RIS
TY - JOUR
TI - Decoupling the effects of surface morphology and interfacial chemistry on localized electrochemical kinetics in LiCoO2 cathodes
AU - Yuxia Guan
AU - Pingshi Wang
AU - Ning Gao
AU - Penghui Liu
AU - Weiwei Cao
AU - Shujiang Ding
AU - Lingjie Meng
AU - Kai Xi
AU - Rui Gao
PY - 2026
DA - 2026/09/09
JO - Chemical Science
DO - 10.1039/d6sc06380b
UR - https://doi.org/10.1039/d6sc06380b
AB - Spatial heterogeneity at electrode/electrolyte interfaces critically influences the electrochemical performance and degradation of lithium-ion batteries, yet the respective contributions of surface morphology and interfacial chemistry to localized electrochemical kinetics remain difficult to distinguish experimentally. Existing characterization techniques reveal either material structural transformation or chemical reconstruction but cannot quantitatively decouple their individual effects on local electrochemical behaviour. Herein, we establish a correlative multimodal strategy by integrating scanning electrochemical cell microscopy (SECCM), atomic force microscopy (AFM), Raman spectroscopy, and finite-element modelling to investigate the spatiotemporal evolution of LiCoO2 thin films during environmental exposure. Spatially resolved SECCM measurements reveal distinct microdomain-dependent electrochemical heterogeneity despite the initially homogeneous structure of the films. Correlative structural and chemical analyses, together with quantitative simulations, demonstrate that surface morphology and interfacial chemistry govern distinct aspects of the electrochemical response. By independently introducing the roughness factor and the effective lithium-ion diffusion coefficient into the multiphysics model, these two contributions can be quantitatively decoupled, with morphology predominantly determining the current response amplitude and interfacial chemistry governing kinetic limitations. This work provides a distinct strategy for correlating local interfacial evolution with electrochemical function and offers new insights into heterogeneous electrochemical interfaces in advanced energy-storage materials.
SN - 2041-6520
SN - 2041-6539
ER -