Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy

Byong-June Lee, Chen Zhao, Jeong-Hoon Yu, Tong-Hyun Kang, Hyean-Yeol Park, Joonhee Kang, Yongju Jung, Xiang Liu, Tianyi Li, Wenqian Xu, Xiao-Bing Zuo, Gui-Liang Xu (), Khalil Amine () and Jong-Sung Yu ()
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Byong-June Lee: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Chen Zhao: Argonne National Laboratory
Jeong-Hoon Yu: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Tong-Hyun Kang: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Hyean-Yeol Park: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Joonhee Kang: Pusan National University
Yongju Jung: Korea University of Technology and Education (KOREATECH)
Xiang Liu: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Wenqian Xu: Argonne National Laboratory
Xiao-Bing Zuo: Argonne National Laboratory
Gui-Liang Xu: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory
Jong-Sung Yu: Daegu Gyeongbuk Institute of Science & Technology (DGIST)

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm−2 (for a total sulfur mass loading of 10 mg cm−2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g−1 and 25 °C.

Date: 2022
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DOI: 10.1038/s41467-022-31943-8

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