In Situ Li3 PS4 Solid-State Electrolyte Protection Layers for Superior Long-Life and High-Rate Lithium-Metal Anodes

Jianwen Liang; Xiaona Li; Yang Zhao; Lyudmila V Goncharova; Gongming Wang; Keegan R Adair; Changhong Wang; Ruying Li; Yongchun Zhu; Yitai Qian; Li Zhang; Rong Yang; Shigang Lu; Xueliang Sun

doi:10.1002/adma.201804684

In Situ Li₃ PS₄ Solid-State Electrolyte Protection Layers for Superior Long-Life and High-Rate Lithium-Metal Anodes

Adv Mater. 2018 Nov;30(45):e1804684. doi: 10.1002/adma.201804684. Epub 2018 Oct 1.

Authors

Jianwen Liang¹, Xiaona Li^{1

2}, Yang Zhao¹, Lyudmila V Goncharova³, Gongming Wang², Keegan R Adair¹, Changhong Wang¹, Ruying Li¹, Yongchun Zhu², Yitai Qian², Li Zhang⁴, Rong Yang⁴, Shigang Lu⁴, Xueliang Sun¹

Affiliations

¹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9, Canada.
² Hefei National Laboratory for Physical Science at Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
³ Department of Physics and Astronomy, University of Western Ontario, London, Ontario, N6A 3K7, Canada.
⁴ China Automotive Battery Research Institute, 5th Floor, No. 43, Mining Building, North Sanhuan Middle RoadHaidi-an District, Beijing, 100088, P. R. China.

PMID: 30276879
DOI: 10.1002/adma.201804684

Abstract

A thin and adjustable Li₃ PS₄ (LPS) solid-state electrolyte protection layer on the surface of Li is proposed to address the dynamic plating/stripping process of Li metal. The LPS interlayer is formed by an in situ and self-limiting reaction between P₄ S₁₆ and Li in N-methyl-2-pyrrolidone. By increasing the concentration of P₄ S₁₆ , the thickness of the LPS layer can be adjusted up to 60 nm. Due to the high ionic conductivity and low electrochemical activity of Li₃ PS₄ , the intimate protection layer of LPS can not only prevent the formation of Li dendrites, but also reduces parasitic side reactions and improves the electrochemical performance. As a result, symmetric cells with the LPS protection layer can deliver stable Li plating/stripping for 2000 h. Full cells assembled with the LPS-protected Li exhibit two times higher capacity retention in Li-S batteries (≈800 mAh g^-1 ) at 5 A g^-1 for over 400 cycles compared to their bare Li counterparts. Furthermore, high rate performances can be achieved with Li-LPS/LiCoO₂ cells, which are capable of cycling at rates as high as 20 C. This innovative and scalable approach to stabilizing the Li anode can serve as a basis for the development of next-generation high-performance lithium-metal batteries.

Keywords: Li3PS4; lithium batteries; lithium-metal anodes; solid-state electrolytes; surface isolation layer.

Abstract

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