Journal
ADVANCED ENERGY MATERIALS
Volume 10, Issue 4, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201903186
Keywords
anode materials; antimony; batteries; catalytic decomposition; solid-electrolyte interphase
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Funding
- National Natural Science Foundation of China [21403157, 21773176]
- Fundamental Research Funds for the Central Universities [2042017kf0232, 2042019kf0200]
- National Science Foundation [CBET1408751]
- U.S. Department of Energy (DOE), Vehicle Technologies Office
- U. S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Clean Vehicles, US-China Clean Energy Research Centre (CERC-CVC2)
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Alloy materials such as Si and Ge are attractive as high-capacity anodes for rechargeable batteries, but such anodes undergo severe capacity degradation during discharge-charge processes. Compared to the over-emphasized efforts on the electrode structure design to mitigate the volume changes, understanding and engineering of the solid-electrolyte interphase (SEI) are significantly lacking. This work demonstrates that modifying the surface of alloy-based anode materials by building an ultraconformal layer of Sb can significantly enhance their structural and interfacial stability during cycling. Combined experimental and theoretical studies consistently reveal that the ultraconformal Sb layer is dynamically converted to Li3Sb during cycling, which can selectively adsorb and catalytically decompose electrolyte additives to form a robust, thin, and dense LiF-dominated SEI, and simultaneously restrain the decomposition of electrolyte solvents. Hence, the Sb-coated porous Ge electrode delivers much higher initial Coulombic efficiency of 85% and higher reversible capacity of 1046 mAh g(-1) after 200 cycles at 500 mA g(-1), compared to only 72% and 170 mAh g(-1) for bare porous Ge. The present finding has indicated that tailoring surface structures of electrode materials is an appealing approach to construct a robust SEI and achieve long-term cycling stability for alloy-based anode materials.
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