Haldar, Sattwick;
Waentig, Albrecht L;
Ramuglia, Anthony R;
Bhauriyal, Preeti;
Khan, Arafat H;
Pastoetter, Dominik L;
Isaacs, Mark A;
... Kaskel, Stefan; + view all
(2023)
Covalent Trapping of Cyclic-Polysulfides in Perfluorinated Vinylene-Linked Frameworks for Designing Lithium-Organosulfide Batteries.
ACS Energy Letters
, 8
pp. 5098-5106.
10.1021/acsenergylett.3c01548.
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Abstract
The strategic combination of redox-active triazine- or quinoxaline-based lithium-ion battery (LIB) mechanisms with the polysulfide ring-mediated lithium-sulfur battery (Li-SB) mechanism enabled the configuration of covalent organic-framework (COF)-derived lithium-organosulfide (Li-OrSB) battery systems. Two vinylene-linked frameworks were designed by enclosing polysulfide rings via postsynthetic framework sulfurization, allowing for the separate construction of triazine-polysulfide and quinoxaline-polysulfide redox couples that can readily interact with Li ions. The inverse vulcanization of the vinylene linking followed by the sulfurization-induced nucleophilic aromatic substitution reaction (SNAr) on the perfluorinated aromatic center of the COFs enabled the covalent trapping of cyclic-polysulfides. The experimentally observed reversible Li-interaction mechanism of these highly conjugated frameworks was computationally verified and supported by in situ Raman studies, demonstrating a significant reduction of polysulfide shuttle in a conventional Li-SB and opening the door for a COF-derived high-performing Li-OrSB.
| Type: | Article |
|---|---|
| Title: | Covalent Trapping of Cyclic-Polysulfides in Perfluorinated Vinylene-Linked Frameworks for Designing Lithium-Organosulfide Batteries |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acsenergylett.3c01548 |
| Publisher version: | https://doi.org/10.1021/acsenergylett.3c01548 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10183062 |
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