期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 42, 页码 47490-47502出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c12873
关键词
silicon anode; hierarchy design; high areal capacity; energy density; prelithiated electrode; operando XRD
资金
- National Natural Science Foundation of China [51602261, 51711530037]
- State Key Laboratory of Solidification Processing (NWPU), China [160-QP-2016]
- Natural Science Foundation of Shaanxi Province, China [2018JM5116]
- University Association for Science and Technology in Shaanxi, China
- Fundamental Research Funds for the Central Universities [3102019JC005]
- Key R&D Program of Shanxi [2019ZDLGY04-05]
Si anodes suffer from poor cycling efficiency because of the pulverization induced by volume expansion, lithium trapping in Li-Si alloys, and unfavorable interfacial side reactions with the electrolyte; the comprehensive consideration of the Si anode design is required for their practical deployment. In this article, we develop a cabbage-inspired graphite scaffold to accommodate the volume expansion of silicon particles in interplanar spacing. With further interfacial modification and prelithiation processing, the Si@G/C anode with an areal capacity of 4.4 mA h cm(-2) delivers highly reversible cycling at 0.5 C (Coulombic efficiency of 99.9%) and a mitigated volume expansion of 23%. Furthermore, we scale up the synthetic strategy by producing 10 kg of the Si@G/C composite in the pilot line and pair this anode with a LiNi0.8Co0.1Mn0.1O2 cathode in a 1 A h pouch-type cell. The full-cell prototype realizes a robust cyclability over 500 cycles (88% capacity retention) and an energy density of 301.3 W h kg(-1) at 0.5 C. Considering the scalable fabrication protocol, holistic electrode formulation design, and harmony integration of key metrics evaluated both in half-cell and full-cell tests, the reversible cycling of the prelithiated silicon species in the graphite scaffold of the composite could enable feasible use of the composite anode in high-energy density lithium batteries.
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