Deep Eutectic Solvent Binder Facilitating Reaction Kinetics of Lithium Sulfur Batteries

C Chen Li (Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY, USA.) Z Zhaokun Wang (Drug Discovery and Design Center, State Key Laboratory of Drug Research, Shanghai Institute of Materia Medica, Chinese Academy of Sciences) Z Zuohang Li (State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) J Junshi Zhang S Su Wang Y Yue Ma X Xixi Shi (State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) H Hongzhou Zhang D Dawei Song (State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) J Jinshi Zhao (State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) L Lianqi Zhang (State Key Laboratory of Crystal Materials, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering)

Abstract

Abstract Existing binders fail to integrate all designed functionalities, including the polysulfide shuttle effect, sluggish kinetic transformation, electrode volume variation, slow Li⁺ transfer, and flammable characteristics. Herein, the microwave irradiation method is used to prepare deep eutectic solvent (DES) binder; with the rapid conduction and full utilization of energy, citric acid and betaine (CB) binder is formed in a flash. Intramolecular and intermolecular hydrogen bonds between C and B provide robust adhesion, self‐healing capability, and flame‐retardant properties. More importantly, Li⁺ flux is directly improved by hydrogen bond acceptor (B) of DES rather than introducing additional segments or chemical treatment; then the redox kinetics are significantly promoted and the polysulfide shuttle is further suppressed. The types and dynamics of the hydrogen bonds are observed via Raman and dynamic mechanical analysis, while effective LiPS adsorption capability is confirmed through theoretical calculations and in situ Raman measurements. Furthermore, rapid LiPS conversion is verified by nucleation/dissolution experiments of Li 2 S and distribution of relaxation times (DRTs) analysis, and nucleation transformation ratio ( NTR ) calculation shows the similar result. Benefiting from the superior merits of the DES binder, lithium–sulfur (Li─S) battery presents stable cycling at 5 C with 61.3% capacity retention after 300 cycles.

Article Details

Volume / Issue Vol. 64, Issue 39
Published September 22, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (11)

C

Chen Li

Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY, USA.

Z

Zhaokun Wang

Drug Discovery and Design Center, State Key Laboratory of Drug Research, Shanghai Institute of Materia Medica, Chinese Academy of Sciences

Z

Zuohang Li

State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

J

Junshi Zhang

S

Su Wang

Y

Yue Ma

X

Xixi Shi

State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

H

Hongzhou Zhang

D

Dawei Song

State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

J

Jinshi Zhao

State Key Laboratory of Crystal Materials School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

L

Lianqi Zhang

State Key Laboratory of Crystal Materials, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering