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Energy Landscapes for Lithium Incorporation and Diffusion in Multidomain Silicon Suboxide Anode Materials
- Title
- Energy Landscapes for Lithium Incorporation and Diffusion in Multidomain Silicon Suboxide Anode Materials
- Authors
- Chae, Somin; Lim, Hyung-Kyu; Lee, Sangheon
- Ewha Authors
- 이상헌
- SCOPUS Author ID
- 이상헌
- Issue Date
- 2023
- Journal Title
- ACS APPLIED MATERIALS & INTERFACES
- ISSN
- 1944-8244
1944-8252
- Citation
- ACS APPLIED MATERIALS & INTERFACES vol. 15, no. 49, pp. 57059 - 57069
- Keywords
- lithium-ion battery; silicon suboxide; Si/SiO2 interface; phase separation; initial Coulombicefficiency; diffusion; density functional theory
- Publisher
- AMER CHEMICAL SOC
- Indexed
- SCIE; SCOPUS
- Document Type
- Article
- Abstract
- 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.
- DOI
- 10.1021/acsami.3c12846
- Appears in Collections:
- 공과대학 > 화공신소재공학과 > Journal papers
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