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Fluorinated Covalent Organic Polymers for High Performance Sulfur Cathodes in Lithium-Sulfur Batteries

Cited 60 time in Web of Science Cited 63 time in Scopus
Authors

Shin, Hyuksoo; Kim, Doyun; Kim, Hyeon Jin; Kim, Jiheon; Char, Kookheon; Yavuz, Cafer T.; Choi, Jang Wook

Issue Date
2019-10
Publisher
American Chemical Society
Citation
Chemistry of Materials, Vol.31 No.19, pp.7910-7921
Abstract
Lithium-sulfur (Li-S) batteries by far offer higher theoretical energy density than that of the commercial lithium-ion battery counterparts, but suffer predominantly from an irreversible shuttling process involving lithium polysulfides. Here, we report a fluorinated covalent organic polymer (F-COP) as a template for high performance sulfur cathodes in Li-S batteries. The fluorination allowed facile covalent attachment of sulfur to a porous polymer framework via nucleophilic aromatic substitution reaction (SNAr), leading to high sulfur content, e.g., over 70 wt %. The F-COP framework was microporous with 72% of pores within three well-defined pore sizes, viz. 0.58, 1.19, and 1.68 nm, which effectively suppressed polysulfide dissolution via steric and electrostatic hindrance. As a result of the structural features of the F-COP, the resulting sulfur electrode exhibited high electrochemical performance of 1287.7 mAh g(-1) at 0.05C, 96.4% initial Columbic efficiency, 70.3% capacity retention after 1000 cycles at 0.5C, and robust operation for a sulfur loading of up to 4.1 mg(sulfur )cm(-2). Our findings suggest the F-COP family with the adaptability of SNAr chemistry and well-defined microporous structures as useful frameworks for highly sustainable sulfur electrodes in Li-S batteries.
ISSN
0897-4756
URI
https://hdl.handle.net/10371/164702
DOI
https://doi.org/10.1021/acs.chemmater.9b01986
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