Journal
NANO LETTERS
Volume 16, Issue 9, Pages 5815-5822Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b02581
Keywords
Nanotube; lithium-ion batteries; in situ TEM electrochemical testing; surface coating; volume expansion; mechanical confinement
Categories
Funding
- NSF [CMMI 1100205, DMR 1410936]
- Chinese 1000-Youth-Talent Plan
- China Scholarship Council
- Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231, 6951379]
- DOE's Office of Biological and Environmental Research
- DOE [DE-AC05-76RLO1830]
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Electrochemically induced mechanical degradation hinders the application of Si anodes in advanced lithium-ion batteries. Hollow structures and surface coatings have been often used to mitigate the degradation, of Si-based anodes. However, the structural change and degradation mechanism during lithiation/delithiation of hollow Si structures with coatings remain unclear. Here, we combine in situ TEM experiment and chemomechanical modeling tri-study the electrochemically induced swelling of amorphous-Si (a-Si) nanotubes with different thicknesses of surface SiOx layers. Surprisingly; we find that no inward expansion occurs at the inner surface during lithiation of a-Si nanotubes with native oxides. In contrast, inward expansion can be induced by increasing the thickness of SiOx on the outer surface, thus reducing the overall outward swelling of the lithiated nanotube. Moreover, both the sandwich lithiation mechanism and the two-stage lithiation process in a Si nanotubes remain unchanged with the-increasing thickness of surface coatings. Our chemomechanical Modeling reveals, the mechanical confinement effects in lithiated a-Si nanotubes with and without SiOx coatings: This work-not only provides insights into the degradation of nanotube anodes with surface coatings but also sheds light onto the optimal design of hollow anodes for high-performance lithium-ion batteries.
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