Highly Reversible Positive-Valence Conversion of Sulfur Chemistry for High-Voltage Zinc-Sulfur Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 38862392.
- Also identified by DOI 10.1002/adma.202402898.
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Abstract
Sulfur is a promising conversion-type cathode for zinc batteries (ZBs) due to its high discharge capacity and cost-effectiveness. However, the redox conversion of multivalent S in ZBs is still limited, only having achieved S<sup>0</sup>/S<sup>2-</sup> redox conversion with low discharge voltage and poor reversibility. This study presents significant progress by demonstrating, for the first time, the reversible S<sup>2-</sup>/S<sup>4+</sup> redox behavior in ZBs with up to six-electron transfer (with an achieved discharge capacity of ≈1284 mAh g<sup>-1</sup>) using a highly concentrated ClO<sub>4</sub> <sup>-</sup>-containing electrolyte. The developed succinonitrile-Zn(ClO<sub>4</sub>)<sub>2</sub> eutectic electrolyte stabilizes the positive-valence S compound and contributes to an ultra-low polarization voltage. Notably, the achieved flat discharge plateaus demonstrate the highest operation voltage (1.54 V) achieved to date in Zn‖S batteries. Furthermore, the high-voltage Zn‖S battery exhibits remarkable conversion dynamics, excellent cycling performance (85.7% capacity retention after 500 cycles), high efficiency (98.4%), and energy density (527 Wh kg <sub>S</sub> <sup>-1</sup>). This strategy of positive-valence conversion of sulfur represents a significant advancement in understanding sulfur chemistry in batteries and holds promise for future high-voltage sulfur-based batteries.