Insights into the Li Diffusion Mechanism in Si/C Composite Anodes for Lithium-Ion Batteries

Gao, Xiang; Lu, Wenquan; Xu, Jun

doi:10.1021/acsami.1c03366

Insights into the Li Diffusion Mechanism in Si/C Composite Anodes for Lithium-Ion Batteries

Journal Article · Fri Apr 30 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c03366· OSTI ID:1798202

Gao, Xiang ^[1]; Lu, Wenquan ^[2]; ^[1]

Univ. of North Carolina, Charlotte, NC (United States); Univ. of North Carolina, Charlotte, NC (United States). North Carolina Motorsports and Automotive Research Center, Vehicle Energy & Safety Lab. (VESL)
Argonne National Lab. (ANL), Lemont, IL (United States)

Recently, Si/C composite materials have attracted enormous research interest as the most promising candidates for the anodes of next-generation lithium-ion batteries, owing to their high energy density and mechanical buffering property. However, the fundamental mechanism of Li diffusion behavior in various Si/C composite materials remains unclear, with our understanding limited by experimental techniques and continuum modeling methodologies. Herein, the atomic behavior of Li diffusion in the Si/C composite material is studied within the framework of density functional theory. Two representative structural mixing formats, that is, simple mixture mode and core-shell mode, are modeled and compared. We discover that the carbon material increases Li diffusion in silicon from 7.75 x 10^-5 to 2.097 x 10^-4 cm²/s. The boost is about 50% more obvious in the mixture mode, while the core-shell structure shows more dependence on the atomic structures of the carbon layer. These results offer new insights into Li diffusion behavior in Si/C composites and unlock the enhancing mechanism for Li diffusion in Si/C. Furthermore, this understanding facilitates the modeling of batteries with composite anodes and will guide the corresponding structure designs for robust and high-energy-density batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1798202

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 18 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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