Energy Landscapes for Lithium Incorporation and Diffusion in Multidomain Silicon Suboxide Anode Materials
- 주제(키워드) lithium-ion battery , silicon suboxide , Si/SiO2 interface , phase separation , initial Coulombicefficiency , diffusion , density functional theory
- 주제(기타) Nanoscience & Nanotechnology; Materials Science, Multidisciplinary
- 설명문(일반) [Chae, Somin; Lee, Sangheon] Ewha Womans Univ, Dept Chem Engn & Mat Sci, Seoul 03760, South Korea; [Chae, Somin; Lee, Sangheon] Ewha Womans Univ, Grad Program Syst Hlth Sci & Engn, Seoul 03760, South Korea; [Lim, Hyung-Kyu] Kangwon Natl Univ, Dept Chem Engn, Chunchon 24341, Gangwon, South Korea
- 관리정보기술 faculty
- 등재 SCIE, SCOPUS
- 발행기관 AMER CHEMICAL SOC
- 발행년도 2023
- URI http://www.dcollection.net/handler/ewha/000000213669
- 본문언어 영어
- Published As https://doi.org/10.1021/acsami.3c12846
- PubMed 38015616
초록/요약
In-depth understanding of the lithium interaction characteristics within multidomain silicon suboxide is indispensable for optimizing the electrochemical performance of silicon suboxide anode materials for lithium-ion batteries. In this study, we investigate the domain-dependent thermodynamic and kinetic properties of lithium atoms within systematically designed multidomain silicon suboxide models composed of Si, SiO2, and Si/SiO2 interface by performing a series of computational simulations combined with a unique tomography-like sampling scheme. We find that the Si/SiO2 interfacial region exhibits preferential thermodynamics and kinetics for lithiation and can serve as a critical lithium transport channel during charge-discharge cycles, while the SiO2 domain is likely to be excluded from lithiation due to its high resistance to lithium diffusion. Consequently, a significant fraction of lithium is expected to be trapped at the Si/SiO2 interface during the discharge process, which ultimately contributes to a low initial Coulombic efficiency. This theoretical understanding suggests that the formation of continuously connected lithium-transportable Si/SiO2 interfacial channels surrounding the Si domains, along with a well-structured shallow SiO2 framework through the use of appropriate synthesis methods, is essential for maximizing the electrochemical performance of silicon suboxide anode materials.
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