Unravelling electro-chemo-mechanical processes in graphite/silicon composites for designing nanoporous and microstructured battery electrodes

Silicon is a promising negative electrode material for high-energy batteries, but its volume changes during cell cycling cause rapid degradation, limiting its loading to about 10 wt.% in conventional graphite/Si composite electrodes. Overcoming this threshold requires evidence-based design for the formulation of advanced electrodes. Here we combine multimodal operando imaging techniques, assisted by structural and electrochemical characterizations, to elucidate the multiscale electro-chemo-mechanical processes in graphite/Si composite negative electrodes. We demonstrate that the electrochemical cycling stability of Si particles strongly depends on the design of intraparticle nanoscale porous structures, and the encapsulation and loss of active Si particles result in excessive charging current being directed to the graphite particles, increasing the risk of lithium plating. We also show that heterogeneous strains are present between graphite and Si particles, in the carbon-binder domain and the electrode's porous structures. Focusing on the volume expansion of the electrode during electrochemical cycling, we prove that the rate performance and Si utilization are heavily influenced by the expansion of the carbon-binder domain and the decrease in porosity. Based on this acquired knowledge, we propose a tailored double-layer graphite/Si composite electrode design that exhibits lower polarization and capacity decay compared with conventional graphite/Si electrode formulations.

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Publication Details

Journal
Nature Nanotechnology
Published
2025-10-24
DOI
https://doi.org/10.1038/s41565-025-02027-7
Citations
6
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
4.38

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article

Unravelling electro-chemo-mechanical processes in graphite/silicon composites for designing nanoporous and microstructured battery electrodes

Xuekun Lu, Antonio Bertei, Daqing Li, Alice V. Llewellyn et al.
6 citations
Nature Nanotechnology
Advancements in Battery Materials
4.38
article

Unravelling electro-chemo-mechanical processes in graphite/silicon composites for designing nanoporous and microstructured battery electrodes

Xuekun Lu, Antonio Bertei, Daqing Li, Alice V. Llewellyn, Han Zhang, Xuhui Yao, Francesco Iacoviello, Jianuo Chen, Shashidhara Marathe, Paul Robert Shearing, Rhodri E. Owen, Christoph Daniel Rau, Xun Zhang, Yunlong Zhao, Wenjia Du, Roby Soni, Qi Li, Zhenyu Zhang
article en
6 citations

Abstract

Silicon is a promising negative electrode material for high-energy batteries, but its volume changes during cell cycling cause rapid degradation, limiting its loading to about 10 wt.% in conventional graphite/Si composite electrodes. Overcoming this threshold requires evidence-based design for the formulation of advanced electrodes. Here we combine multimodal operando imaging techniques, assisted by structural and electrochemical characterizations, to elucidate the multiscale electro-chemo-mechanical processes in graphite/Si composite negative electrodes. We demonstrate that the electrochemical cycling stability of Si particles strongly depends on the design of intraparticle nanoscale porous structures, and the encapsulation and loss of active Si particles result in excessive charging current being directed to the graphite particles, increasing the risk of lithium plating. We also show that heterogeneous strains are present between graphite and Si particles, in the carbon-binder domain and the electrode's porous structures. Focusing on the volume expansion of the electrode during electrochemical cycling, we prove that the rate performance and Si utilization are heavily influenced by the expansion of the carbon-binder domain and the decrease in porosity. Based on this acquired knowledge, we propose a tailored double-layer graphite/Si composite electrode design that exhibits lower polarization and capacity decay compared with conventional graphite/Si electrode formulations.

Nature NanotechnologyVol. 20(11)
University of Pisa (IT), National Physical Laboratory (GB), Queen Mary University of London (GB), University of Exeter (GB), Biochemical Society (GB), Diamond Light Source (GB), University of Manchester (GB), Henry Royce Institute (GB), Beijing University of Technology (CN), University of Warwick (GB), University of Oxford (GB), The London College (GB), The Faraday Institution (GB), University College London (GB), Imperial College London (GB)
Royal Academy of Engineering, Engineering and Physical Sciences Research Council
Openalex Percentile: Top 5%
Advancements in Battery Materials
4.38
DOIOpen Access PDFOpenAlex
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