Unraveling the Catalyst-Solvent Interactions in Lean-Electrolyte Sulfur Reduction Electrocatalysis for Li-S Batteries

Angew Chem Int Ed Engl. 2022 Dec 19;61(51):e202213863. doi: 10.1002/anie.202213863. Epub 2022 Nov 22.

Abstract

Efficient catalyst design is important for lean-electrolyte sulfur reduction in Li-S batteries. However, most of the reported catalysts were focused on catalyst-polysulfide interactions, and generally exhibit high activity only with a large excess of electrolyte. Herein, we proposed a general rule to boost lean-electrolyte sulfur reduction by controlling the catalyst-solvent interactions. As evidenced by synchrotron-based analysis, in situ spectroscopy and theoretical computations, strong catalyst-solvent interaction greatly enhances the lean-electrolyte catalytic activity and battery stability. Benefitting from the strong interaction between solvent and cobalt catalyst, the Li-S battery achieves stable cycling with only 0.22 % capacity decay per cycle with a low electrolyte/sulfur mass ratio of 4.2. The lean-electrolyte battery delivers 79 % capacity retention compared with the battery with flooded electrolyte, which is the highest among the reported lean-electrolyte Li-S batteries.

Keywords: Catalyst-Solvent Interactions; Electrocatalysis; Lean Electrolyte Condition; Li−S Batteries; Sulfur Reduction Reaction.