Sulfide-Bridged Covalent Quinoxaline Frameworks for Lithium–Organosulfide Batteries

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

Abstract

The chelating ability of quinoxaline cores and the redox activity of organosulfide bridges in layered covalent organic frameworks (COFs) offer dual active sites for reversible lithium (Li)-storage. The designed COFs combining these properties feature disulfide and polysulfide-bridged networks showcasing an intriguing Li-storage mechanism, which can be considered as a lithium–organosulfide (Li–OrS) battery. The experimental–computational elucidation of three quinoxaline COFs containing systematically enhanced sulfur atoms in sulfide bridging demonstrates fast kinetics during Li interactions with the quinoxaline core. Meanwhile, bilateral covalent bonding of sulfide bridges to the quinoxaline core enables a redox-mediated reversible cleavage of the sulfur-sulfur bond and the formation of covalently anchored lithium–sulfide chains or clusters during Li-interactions, accompanied by a marked reduction of Li–polysulfide (Li–PS) dissolution into the electrolyte, a frequent drawback of lithium–sulfur (Li–S) batteries. The electrochemical behavior of model compounds mimicking the sulfide linkages of the COFs and operando Raman studies on the framework structure unravels the reversibility of the profound Li-ion–organosulfide interactions. Thus, integrating redox-active organic-framework materials with covalently anchored sulfides enables a stable Li–OrS battery mechanism which shows benefits over a typical Li–S battery.

Details

Original languageEnglish
Article number2210151
Number of pages14
JournalAdvanced materials
Volume35
Issue number16
Publication statusPublished - 13 Mar 2023
Peer-reviewedYes

External IDs

WOS 000948354700001

Keywords

Keywords

  • 2D materials, covalent organic frameworks, mechanism studies, sulfide batteries, Covalent organic frameworks, Mechanism studies, Sulfide batteries