Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 8, Pages 4322-4328Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202013264
Keywords
high capacity; organosulfide; redox chemistry; redox flow batteries; resonance structure
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Funding
- Exxon Mobil Corp.
- Sloan Research Fellowship
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The study demonstrates the effectiveness of using organosulfides as a new model material system to design redox-active molecules in nonaqueous systems. The TETD molecule shows high solubility and reversible capacity in various organic solvents, along with high electrochemical stability in different organic electrolytes. Material/structural characterizations reveal the underlying mechanism of redox chemistry in organodisulfides involving the cleavage and reformation of disulfide bonds.
Nonaqueous redox flow batteries (RFBs) have great potential to achieve high-energy storage systems. However, they have been limited by low solubility and poor stability of active materials. Here we demonstrate organosulfides as a new-type model material system to explore the rational design of redox-active molecules in nonaqueous systems. The tetraethylthiuram disulfide (TETD) molecule shows high solubility in various common organic solvents and achieves a high reversible capacity of ca. 50 Ah L-1 at a high concentration of 1 M. The resonance structures in the reduced product endow the molecule with high electrochemical stability in different organic electrolytes. The underlying mechanism in redox chemistry of organodisulfides involving the cleavage and reformation of disulfide bonds is revealed by material/structural characterizations. This study provides a new perspective of molecule designs for the development of redox-active materials for high-performance nonaqueous RFBs.
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