Physicochemical Heterogeneity in Silicon Anodes from Cycled Lithium-Ion Cells
[1];
[2];
[3];
[4];
[3]
- Univ. of Illinois at Urbana-Champaign, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Illinois Institute of Technology, Chicago, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Illinois at Urbana-Champaign, IL (United States)
The severe capacity fade of lithium-ion cells with silicon-dominant anodes has hindered their widescale commercialization. In this work, we link cell capacity fade to the heterogeneous physicochemical evolution of silicon anodes during battery cycling. Through a multi-length scale characterization approach, we demonstrate that silicon particles near the anode surface react differently than those near the copper current collector. In particular, near the anode surface we find an amorphized wispy silicon encased in a highly fluorinated matrix of electrolyte-reduction products. In contrast, closer to the current collector, the silicon retains more of its initial morphology and structure, suggesting the presence of isolated particles. Here, the results show that accessibility of active silicon to lithium-ions varies across the anode matrix. Material and cell designs, which minimize electrode expansion resulting from the in-filling of pores with the solid electrolyte interphase (SEI), are needed to enhance anode homogeneity during the electrochemical cycling.
- Research Organization:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- Grant/Contract Number:
- AC02-06CH11357; SC0014664
- OSTI ID:
- 1962362
- Journal Information:
- ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 34 Vol. 14; ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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