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

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

Research output: Contribution to journalArticlepeer-review

16 Citations (Scopus)


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.

Original languageEnglish
Pages (from-to)31733-31740
Number of pages8
JournalACS Applied Materials and Interfaces
Issue number27
Publication statusPublished - 2021 Jul 14

Bibliographical note

Funding Information:
The work done at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE, through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract DE-SC0012704. This research used beamline 8-BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. The work done at UC San Diego was supported by the Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) under contract no. DE-EE0007764. Part of the work used the UCSD-MTI Battery Fabrication Facility and the UCSD-Arbin Battery Testing Facility.

Publisher Copyright:
© 2021 American Chemical Society.

All Science Journal Classification (ASJC) codes

  • Materials Science(all)


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