期刊
ACS NANO
卷 13, 期 9, 页码 10671-10681出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b05029
关键词
copper tin sulfide; gelation-solvothermal; in situ X-ray diffraction; density functional theory; diffusion kinetic; thin-film lithium battery
类别
资金
- Welch Foundation [F-1131, F-1841, F-1436]
- National Science Foundation [CBET-1603491]
- China Scholarship Council (CSC) scholarship under the State Scholarship Fund
Through a simple gelation-solvothermal method with graphene oxide as the additive, a Cu4SnS4-rich composite of nanoparticles and nanotubes is synthesized and applied for thin and flexible Li-metal batteries. Unlike the Cu2SnS3-rich electrode, the Cu4SnS4-rich electrode cycles stably with an enhanced conversion capacity of similar to 416 mAh g(-1) (similar to 52% of total capacity) after 200 cycles. The lithiation/delithiation mechanisms of Cu-Sn-S electrodes and the voltage ranges of conversion and alloying reactions are informed by in situ X-ray diffraction tests. The conversion process of three Cu-Sn-S compounds is compared by density functional theory (DFT) calculations based on three algorithms, elucidating the enhanced conversion stability and superior diffusion kinetics of Cu4SnS4 electrodes. The reaction pathway of Cu-Sn-S electrodes and the root cause for the unstable capacity are revealed by in situ/ex situ characterizations, DFT calculations, and various electrochemical tests. This work provides insight into developing energy materials and power devices based on multiple lithiation mechanisms.
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