Citation: Fengfeng Han, Lirong Zhang, Qi Jin, Yufei Zhang, Zhiguo Zhang, Liu Liu, Lu Li, Xinzhi Ma, Xitian Zhang, Lili Wu. Strong interaction between high-entropy alloy catalysts and solvent molecules facilitating the polysulfide conversion in lean-electrolyte lithium-sulfur batteries[J]. Chinese Chemical Letters, ;2026, 37(11): 111814. doi: 10.1016/j.cclet.2025.111814 shu

Strong interaction between high-entropy alloy catalysts and solvent molecules facilitating the polysulfide conversion in lean-electrolyte lithium-sulfur batteries

Fengfeng Han ^{a, 1} ,
Lirong Zhang ^{a, 1} ,
Qi Jin ^a ,
Yufei Zhang ^a ,
Zhiguo Zhang ^b ,
Liu Liu ^c ,
Lu Li ^a ,
Xinzhi Ma ^a ,
Xitian Zhang ^{a, *,} ,
Lili Wu ^{a, *,}

a.
Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin 150025, China
b.
Department of Physics, Harbin Institute of Technology, Harbin 150001, China
c.
College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China

xtzhangzhang@hotmail.com

wll790107@hotmail.com

Received Date: 3 July 2025
Revised Date: 1 September 2025
Accepted Date: 9 September 2025
Available Online: 9 September 2025

Figures(7)

The design of an efficient catalyst is crucial for sulfur reduction reaction (SRR) in lean electrolyte lithium-sulfur (Li–S) batteries. However, most existing catalysts primarily focus on polysulfide-catalyst interactions and generally demonstrate high activity only with an excessive electrolyte. In this study, we propose high-entropy alloy (HEA) composite to enhance the SRR under lean-electrolyte conditions by optimizing the solvent-catalyst interaction. As evidenced by in situ spectroscopy, nuclear magnetic resonance (NMR), density functional theory (DFT) calculations, and experimental investigations, the strong interaction between the solvent and HEA catalysts enables the Li–S battery to achieve a high capacity of 1007.9 mAh/g with a low E/S ratio of 10 µL/mg, and capacity retention of 77% after 200 cycles at lower E/S ratio of 4.5 µL/mg. The enhanced SRR performance in lean electrolyte conditions is primarily attributed to d–d electron interactions among the constituent metals and the presence of multiple active sites with optimized energy barriers in the HEA catalysts. This work underscores the significance of solvent-catalyst interactions in regulating the SRR of lean electrolyte Li–S battery and offers insights into the rational design of HEA catalysts to advance Li−S batteries.
- Catalyst-solvent interactions,
- Li–S batteries,
- Lean electrolyte,
- Sulfur reduction reaction,
- High entropy alloy
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