期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 27, 页码 31733-31740出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c07903
关键词
lithium sulfur batteries; sulfurized polyacrylonitrile; Li metal; X-ray fluorescence microscopy; X-ray absorption spectroscopy; lean electrolyte; high energy density
资金
- Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE, through the Advanced Battery Materials Research (BMR) Program, Battery500 Consortium [DE-SC0012704]
- DOE Office of Science [DE-SC0012704]
- Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007764]
The study demonstrates the crucial role of LiNO3 additive in preventing LiSx species from dissolving into the electrolyte, thereby reducing shuttle effect and capacity loss. Carbonate electrolyte forms porous dendritic Li morphology on Li anode, while ether-based electrolyte forms dense spherical Li morphology, proving that ether-based electrolyte with LiNO3 is the preferred choice for stable cycling.
Sulfurized polyacrylonitrile (SPAN) is a promising high-capacity cathode material. In this work, we use spatially resolved X-ray absorption spectroscopy combined with X-ray fluorescence (XRF) microscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy to examine the structural transformation of SPAN and the critical role of a robust cathode-electrolyte interface (CEI) on the electrode. LiSx species forms during the cycling of SPAN. However, in carbonate-based electrolytes and ether-based electrolytes with LiNO3 additives, these species are well protected by the CEI and do not dissolve into the electrolytes. In contrast, in an ether-based electrolyte without the LiNO3 additive, LiSx species dissolve into the electrolyte, resulting in the shuttle effect and capacity loss. Examination of the Li anode by XRF and SEM reveals dense spherical Li morphology in ether-based electrolytes, but sulfur is present in the absence of the LiNO3 additive. In contrast, porous dendritic Li is found in the carbonate electrolyte. These analyses established that an ether-based electrolyte with LiNO3 is a superior choice that enables stable cycling of both electrodes. Based on these insights, we successfully demonstrate the stable cycling of high areal loading SPAN cathode (>6.5 mA h cm(-2)) with lean electrolyte amounts, showing promising Li.SPAN cell performance under practical conditions.
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