期刊
ADVANCED MATERIALS
卷 32, 期 23, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202000302
关键词
functional composite separators; hybrid electrolytes; in situ interfacial polymerization; lithium-selenium batteries; lithium-sulfur batteries
类别
资金
- National Natural Science Foundation of China [51788104, 21805062, 21975266]
- National Key R&D Program of China [2016YFA0202500, 2019YFA0705700]
- Beijing Natural Science Foundation [L172023]
- Beijing National Laboratory for Molecular Sciences [BNLMS-CXXM-201906]
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA 21070300]
- Recruitment Program of Global Youth Experts of China
- Chinese Academy of Sciences
Lithium-chalcogen batteries are an appealing choice for high-energy-storage technology. However, the traditional battery that employs liquid electrolytes suffers irreversible loss and shuttle of the soluble intermediates. New batteries that adopt Li+-conductive polymer electrolytes to mitigate the shuttle problem are hindered by incomplete discharge of sulfur/selenium. To address the trade-off between energy and cycle life, a new electrolyte is proposed that reconciles the merits of liquid and polymer electrolytes while resolving each of their inferiorities. An in situ interfacial polymerization strategy is developed to create a liquid/polymer hybrid electrolyte between a LiPF6-coated separator and the cathode. A polymer-gel electrolyte in situ formed on the separator shows high Li+ transfer number to serve as a chemical barrier against the shuttle effect. Between the gel electrolyte and the cathode surface is a thin gradient solidification layer that enables transformation from gel to liquid so that the liquid electrolyte is maintained inside the cathode for rapid Li+ transport and high utilization of active materials. By addressing the dilemma between the shuttle chemistry and incomplete discharge of S/Se, the new electrolyte configuration demonstrates its feasibility to trigger higher capacity retention of the cathodes. As a result, Li-S and Li-Se cells with high energy and long cycle lives are realized, showing promise for practical use.
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