A lithium sulfonylimide COF-modified separator for high-performance Li-S batteries
Jie Liu1,3, Jinping Zhang1,3, Jie Zhu1,3, Ruiqi Zhao1,3, Yamin Zhang4, Yanfeng Ma1,3, Chenxi Li1,3, Hongtao Zhang1,3(), Yongsheng Chen1,2,3()
The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin 300071, China
State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin 300071, China
Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin 300071, China
State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China
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A lithium sulfonylimide covalent organic framework (COF) (COF-LiSTFSI, LiSTFSI = lithium (4-styrenesulfonyl) (trifluoromethanesulfonyl)imide) was designed and synthesized to modify the separator for lithium-sulfur (Li-S) batteries, providing a solution for addressing issues of polysulfides shuttle effect and promoting Li+ transport. The batteries using COF-LiSTFSI modified separator exhibit a high capacity of 1229.7 mAh·g−1 at 0.2 C and a low attenuation rate of 0.042% per cycle after 1000 cycles at 1 C.
Abstract
Lithium-sulfur (Li-S) batteries are highly regarded as the next-generation high-energy-density secondary batteries due to their high capacity and large theoretical energy density. However, the practical application of these batteries is hindered mainly by the polysulfide shuttle issue. Herein, we designed and synthesized a new lithium sulfonylimide covalent organic framework (COF) material (COF-LiSTFSI, LiSTFSI = lithium (4-styrenesulfonyl) (trifluoromethanesulfonyl)imide), and further used it to modify the common polypropylene (PP) separator of Li-S batteries. The COF-LiSTFSI with sulfonylimide anion groups features stronger electronegativity, thus can effectively facilitate the lithium ion conduction while significantly suppress the diffusion of polysulfides via the electrostatic interaction. Compared with the unmodified PP separator, the COF-LiSTFSI modified separator results in a high ionic conductivity (1.50 mS·cm−1) and Li+ transference number (0.68). Consequently, the Li-S battery using the COF-LiSTFSI modified separator achieves a high capacity of 1229.7 mAh·g−1 at 0.2 C and a low decay rate of only 0.042% per cycle after 1000 cycles at 1 C, compared with those of 941.5 mAh·g−1 and 0.061% using the unmodified PP separator, respectively. These results indicate that by choosing suitable functional groups, an effective strategy for COF-modified separators could be developed for high-performance Li-S batteries.
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