Understanding the Roles of the Electrode/Electrolyte Interface for Enabling Stable Li∥Sulfurized Polyacrylonitrile Batteries

Wu, Zhaohui; Bak, Seong-Min; Shadike, Zulipiya; Yu, Sicen; Hu, Enyuan; Xing, Xing; Du, Yonghua; Yang, Xiao-Qing; Liu, Haodong; Liu, Ping

doi:10.1021/acsami.1c07903

Understanding the Roles of the Electrode/Electrolyte Interface for Enabling Stable Li∥Sulfurized Polyacrylonitrile Batteries

Journal Article · Fri Jul 02 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c07903· OSTI ID:1807959

^[1]; ^[2]; ^[3]; Yu, Sicen ^[1]; ^[3]; Xing, Xing ^[1]; Du, Yonghua ^[2]; ^[3]; Liu, Haodong ^[1]; ^[1]

Univ. of California, San Diego, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.

Sulfurized polyacrylonitrile (SPAN) is a promising high-capacity cathode material. Here, 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. LiS_x 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, LiS_x 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: EE0007764; SC0012704

OSTI ID:: 1807959

Report Number(s):: BNL--221776-2021-JAAM

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 27 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Understanding the Roles of the Electrode/Electrolyte Interface for Enabling Stable Li∥Sulfurized Polyacrylonitrile Batteries

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