Tuning the Linkers in Polymer-Based Cathodes to Realize High Sulfur Content and High-Performance Potassium–Sulfur Batteries

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Tuning the Linkers in Polymer-Based Cathodes to Realize High Sulfur Content and High-Performance Potassium–Sulfur Batteries

Zhang, L; Ge, L; He, G; Tian, Z; Huang, J; Wang, J; Brett, DJL; ... Liu, T; + view all (2021) Tuning the Linkers in Polymer-Based Cathodes to Realize High Sulfur Content and High-Performance Potassium–Sulfur Batteries. The Journal of Physical Chemistry C , 125 (34) pp. 18604-18613. 10.1021/acs.jpcc.1c05283. Green open access

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Abstract

The development of effective rechargeable potassium–sulfur (K–S) batteries has been retarded by a severe polysulfide shuttle effect and low sulfur content in the cathode (generally less than 40 wt %). Herein, a series of sulfur-linked polymers with different numbers of allyloxy linkers have been chosen to explore their effect on the performance of K–S batteries. By taking sulfur-linked tetra(allyloxy)-1,4-benzoquinone polymer (poly(S4-TABQ)) as the cathode of K–S batteries, its maximal sulfur content reaches ∼71 wt %, which displays a high capacity retention of 94.5% after 200 cycles (only 0.027% loss per cycle). Theoretical analyses and density functional theory calculations show that the abundant allyloxy linkers in poly(S4-TABQ) cathodes play a vital role in inhibiting the polysulfide shuttle effect and realizing high capacity, owing to the strong interaction of the allyloxy moieties with potassium polysulfides and the accelerated charge transfer during charge/discharge process. Moreover, ex situ X-ray photoelectron spectroscopy and ultraviolet–visible spectroscopy analysis are conducted to explore the electrochemical mechanism in poly(S4-TABQ) cathodes, indicating that −C-Sn–·K+ (n = 2–6) and K2Sn (n = 2–6) coexist in K–S batteries without the formation of K2S groups. This study provides a novel insight into the application of sulfur-linked polymers as cathode material in potassium–sulfur batteries.

Type:	Article
Title:	Tuning the Linkers in Polymer-Based Cathodes to Realize High Sulfur Content and High-Performance Potassium–Sulfur Batteries
Open access status:	An open access version is available from UCL Discovery
DOI:	10.1021/acs.jpcc.1c05283
Publisher version:	https://doi.org/10.1021/acs.jpcc.1c05283
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 Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering 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/10140266