Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries

Yubin He, Peichao Zou, Seong Min Bak, Chunyang Wang, Rui Zhang, Libing Yao, Yonghua Du, Enyuan Hu, Ruoqian Lin, Huolin L. Xin

Research output: Contribution to journalArticlepeer-review

9 Citations (Scopus)


The reliability and durability of lithium metal (Li0)-sulfur batteries are largely limited by the undesired Li0plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. Herein, we report the stable operation of a Li0-SPAN (sulfurized polyacrylonitrile) battery via an anode-cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li3N-forming additive (TMS-N3), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li0anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li0plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li2S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/gSPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode-electrolyte interphase engineering strategy has tackled the major limitations of Li-S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from -10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li0-S batteries.

Original languageEnglish
Pages (from-to)2866-2875
Number of pages10
JournalACS Energy Letters
Issue number9
Publication statusPublished - 2022 Sept 9

Bibliographical note

Funding Information:
We at the UCI acknowledge support from the Office of Basic Energy Sciences of the U.S. Department of Energy (DOE), under award no. DE-SC0021204 (for TEM studies) and the startup funding of H.L.X. provided by UC Irvine (for electrochemistry and X-ray studies). The authors acknowledge the use of facilities and instrumentation at the UC Irvine Materials Research Institute (IMRI), which is supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center (DMR-2011967). XPS work was performed using instrumentation funded in part by the National Science Foundation Major Research Instrumentation Program under grant no. CHE-1338173. R.L. and E.H. are supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy, through the Advanced Battery Materials Research (BMR) Program under contract DE-SC0012704. This research used resources of the 8-BM beamline of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

All Science Journal Classification (ASJC) codes

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry


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