期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 16, 页码 18634-18645出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c03461
关键词
lithium-sulfur batteries; functional separator; lithium polysulfides; shuttle effect; CeO2-x; kinetics
资金
- National Natural Science Foundation of China [U1810204, 51972093, 52072104, U1910210]
- Nature Science Foundation of Anhui Province [2008085ME129]
- Key Research and Development Plan of Anhui Province [202004b11020024]
- Fundamental Research Funds for the Central Universities of China [PA2021GDSK0087, PA2020GDSK0088, PA2020GDJQ0026]
The commercialization of high-energy Li-S batteries is limited by their poor cycle retention and cycling life due to lithium polysulfide shuttling. In this study, a multilayered functional CeO2-x@C-rGO/CNT separator was successfully fabricated, which can effectively hinder the diffusion of polysulfide species, accelerate the redox reactions of sulfur species, and enhance the conductivity for sulfur reactivation and efficient utilization. The Li-S battery assembled with this separator demonstrates excellent capacity, rate capability, and cycling performance, as well as reduced self-discharge and anode corrosion.
Commercialization of high-energy Li-S batteries is greatly restricted by their unsatisfactory cycle retention and poor cycling life originated from the notorious shuttling effect of lithium polysulfides. Modification of a commercial separator with a functional coating layer is a facile and efficient strategy beyond nanostructured composite cathodes for suppressing polysulfide shuttling. Herein, a multilayered functional CeO2-x@C-rGO/CNT separator was successfully achieved by alternately depositing conductive carbon nanotubes (CNTs) and synthetic CeO2-x@C-rGO onto the surface of the commercial separator. The cooperation of multiple components including Ce-MOF-derived CeO2-x@C, rGO, and CNTs enables the as-built CeO2-x@C-rGO/CNT separator to perform multifunctions from the separator surface: (i) to hinder the diffusion of polysulfide species through physical blocking or chemical adsorption, (ii) to accelerate the sluggish redox reactions of sulfur species, and (iii) to enhance the conductivity for sulfur reactivation and efficient utilization. Serving as a multilayer and powerful barrier, the CeO2-x@C-rGO/CNT separator greatly constrains and reutilizes the polysulfide species. Thus, the Li-S battery assembled with the CeO2-x@C-rGO/CNT separator demonstrates an excellent combination of capacity, rate capability, and cycling performances (an initial capacity of 1107 mA h g(-1) with a low decay rate of 0.060% per cycle over 500 cycles at 1 C, 651 mA h g(-1) at 5 C) together with remarkably mitigated self-discharge and anode corrosion. This work provides guidelines for functional separator design as well as rare-earth material applications for Li-S batteries and other energy storage systems.
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