journal article·2023-12-08Open access

Covalent Trapping of Cyclic-Polysulfides in Perfluorinated Vinylene-Linked Frameworks for Designing Lithium-Organosulfide Batteries

Sattwick Haldar, Albrecht L. Waentig, Anthony R. Ramuglia, Preeti Bhauriyal, Arafat H. Khan, Dominik L. Pastoetter, Mark A. Isaacs, Ankita De, Eike Brunner, Mingchao Wang, Thomas Heine, Inez M. Weidinger, Xinliang Feng, Andreas Schneemann, Stefan Kaskel

ACS Energy Letters· Volume 8· Issue 12

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 (S N Ar) 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.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Covalent Organic Framework Applications · Advanced Battery Materials and Technologies · Metal-Organic Frameworks: Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Inorganic Chemistry I, Technische Universität Dresden, Dresden 01069, Germany

Center for Advancing Electronics Dresden (cfaed) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01069 Dresden, Germany

Electrochemistry, Technische Universität Dresden, 01069 Dresden, Germany

Theoretical Chemistry, Technische Universität Dresden, 01069 Dresden, Germany

Bioanalytical Chemistry, Technische Universität Dresden, 01069 Dresden, Germany

Department of Chemistry, University College London, London, WC1H 0AJ U.K.

HarwellXPS, Research Complex at Harwell, Rutherford Appleton Laboratories, Didcot, OX11 0FA U.K.

Fraunhofer Institute for Material and Beam Technology (IWS), Winterbergstraße 28, Dresden 01277, Germany

Funding

Deutsche Forschungsgemeinschaft · Fonds der Chemischen Industrie · Alexander von Humboldt-Stiftung

References (36)

Show source-provided references
1. 10.1126/science.aal158510.1126/science.aal1585 ↗
2. 10.1021/acs.chemrev.9b0055010.1021/acs.chemrev.9b00550 ↗
3. 10.1002/adfm.20210050510.1002/adfm.202100505 ↗
4. 10.1002/anie.20230227610.1002/anie.202302276 ↗
5. 10.1016/j.enchem.2020.10004810.1016/j.enchem.2020.100048 ↗
6. 10.1002/pol.2021094010.1002/pol.20210940 ↗
7. 10.1021/jacs.3c0113110.1021/jacs.3c01131 ↗
8. 10.1021/acsami.8b1421310.1021/acsami.8b14213 ↗
9. 10.1021/jacs.2c0234610.1021/jacs.2c02346 ↗
10. 10.1021/acs.energyfuels.2c0103510.1021/acs.energyfuels.2c01035 ↗
11. 10.1002/adma.20221015110.1002/adma.202210151 ↗
12. 10.1039/D1QM00015B10.1039/D1QM00015B ↗
13. 10.1016/j.matt.2020.09.00710.1016/j.matt.2020.09.007 ↗
14. 10.1002/anie.20181268510.1002/anie.201812685 ↗
15. 10.1016/j.ensm.2021.01.01610.1016/j.ensm.2021.01.016 ↗
16. 10.1038/nenergy.2017.7410.1038/nenergy.2017.74 ↗
17. 10.1039/C8TA07008C10.1039/C8TA07008C ↗
18. 10.1002/chem.20210450210.1002/chem.202104502 ↗
19. 10.1002/adfm.20190292910.1002/adfm.201902929 ↗
20. 10.1016/0022-2364(83)90211-110.1016/0022-2364(83)90211-1 ↗
21. 10.1016/j.micromeso.2015.02.02210.1016/j.micromeso.2015.02.022 ↗
22. 10.1016/0009-2614(82)83547-110.1016/0009-2614(82)83547-1 ↗
23. 10.5194/acp-19-8175-201910.5194/acp-19-8175-2019 ↗
24. 10.3390/coatings1007061910.3390/coatings10070619 ↗
25. 10.1021/acsami.9b1470910.1021/acsami.9b14709 ↗
26. 10.1149/2.045308jes10.1149/2.045308jes ↗
27. 10.1002/jrs.452110.1002/jrs.4521 ↗
28. 10.1016/j.ensm.2022.03.01510.1016/j.ensm.2022.03.015 ↗
29. 10.1038/s41467-021-23155-310.1038/s41467-021-23155-3 ↗
30. 10.1149/1945-7111/acb3fe10.1149/1945-7111/acb3fe ↗
31. Frisch M. J. · 2013
32. 10.1016/j.jechem.2023.02.03610.1016/j.jechem.2023.02.036 ↗
33. 10.3390/polym1507168510.3390/polym15071685 ↗
34. 10.1021/acs.jpca.0c0183810.1021/acs.jpca.0c01838 ↗
35. 10.1039/D0NH00187B10.1039/D0NH00187B ↗
36. 10.1021/jacs.5b0811310.1021/jacs.5b08113 ↗