Pinned Electrode/Electrolyte Interphase and Its Formation Origin for Sulfurized Polyacrylonitrile Cathode in Stable Lithium Batteries

Zhang, Xianhui; Gao, Peiyuan; Wu, Zhaohui; Engelhard, Mark H.; Cao, Xia; Jia, Hao; Xu, Yaobin; Liu, Haodong; Wang, Chongming; Liu, Jun; Zhang, Ji-Guang; Liu, Ping; Xu, Wu

doi:10.1021/acsami.2c16890

DOE OSTI · 1901869

Pinned Electrode/Electrolyte Interphase and Its Formation Origin for Sulfurized Polyacrylonitrile Cathode in Stable Lithium Batteries

Zhang, Xianhui·Gao, Peiyuan·Wu, Zhaohui·Engelhard, Mark H.·Cao, Xia·Jia, Hao·Xu, Yaobin·Liu, Haodong·Wang, Chongming·Liu, Jun·Zhang, Ji-Guang·Liu, Ping·Xu, Wu

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Abstract

Sulfurized polyacrylonitrile (SPAN) represents one of the most promising directions for high-energy-density lithium (Li)-sulfur batteries. However, the practical application of Li||SPAN is currently limited by the insufficient chemical/electrochemical stability of electrode/electrolyte interphase (EEI). Here, a pinned EEI layer is designed for stabilizing a SPAN cathode by regulating the EEI formation mechanism in an advanced LiFSI/ether/fluorinated-ether electrolyte. Computational simulations and experimental investigations reveal that, benefiting from the nonsolvating nature, the fluorinated-ether can not only act as a protective shield to prevent the Li polysulfides dissolution but also, more importantly, endow a diffusion-controlled EEI formation process. It promotes the formation of a uniform, protective, and conductive EEI layer pinning into SPAN surface region, enabling the high loading Li||SPAN batteries with superior cycling stability, wide temperature performance, and high-rate capability. Finally, this design strategy opens an avenue for exploring advanced electrolytes for Li||SPAN batteries and guides the interface design for broad types of battery systems.

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25 ENERGY STORAGE Li metal anode electrode/electrolyte interphase high cathode loading lithium-sulfur batteries sulfurized polyacrylonitrile

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Zhang, Xianhui, Gao, Peiyuan, Wu, Zhaohui, Engelhard, Mark H., Cao, Xia, Jia, Hao, Xu, Yaobin, Liu, Haodong, Wang, Chongming, Liu, Jun, Zhang, Ji-Guang, Liu, Ping, Xu, Wu. 2022-11-15. Pinned Electrode/Electrolyte Interphase and Its Formation Origin for Sulfurized Polyacrylonitrile Cathode in Stable Lithium Batteries. https://doi.org/10.1021/acsami.2c16890

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