Robust Interface Enabled by Bicontinuous‐Structured Electrolyte Elastomers for Solid‐State Battery Applications

Q Qing‐Yao Zhu (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China) X Xiao‐Xue Wang (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China) D De‐Hui Guan (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China) J Jian‐You Li (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China) X Xin‐Yuan Yuan (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China) H Huan‐Feng Wang (College of Materials and Chemical Engineering Zhengzhou Key Laboratory of Functional Electrocatalysis and Chemical Energy Storage Zhengzhou University of Technology Zhengzhou 450044 P.R. China) J Ji‐Jing Xu (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China)

Abstract

Abstract Solid‐state electrolytes (SSEs) with high ionic conductivity, superior electrochemical stability, and mechanical durability are safe and reliable for solid‐state lithium (Li) batteries. However, most existing SSEs suffer from limited mechanical resilience and poor interface contact, impeding their practical deployment. Here, an in situ phase separation strategy is proposed to construct a class of elastomeric solid‐state electrolytes with bicontinuous architecture. The rigid phase ensures high ionic conductivity (7.8 × 10 −4 S cm −1 at 25 °C), while the elastic phase provides excellent elastic restorability (82%) and strong interface contact (adhesion energy ≈43.9 J m −2 ). This bicontinuous structure endows the material with superior stretchability (1800%), fatigue resistance, and puncture strength, while maintaining interface contact, keeping mechanical integrity of the battery structure during cycling, and restraining the dendrite growth. Consequently, symmetric batteries exhibit no short‐circuiting even after 2000 h of operation, and Li–metal batteries demonstrate high specific capacity. Solid‐state Li–O 2 batteries fabricated with the P(BA‐SN)‐IL electrolyte also exhibit good cycling performance (500 cycles), and the Li–O 2 pouch cell achieves stable cycling and superior feasibility under various abuse tests, including bending and squeezing. The bicontinuous‐structured elastomer electrolytes present a highly promising strategy for enabling safe operation of high‐energy solid‐state batteries.

Article Details

Volume / Issue Vol. 65, Issue 8
Published February 16, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (7)

Q

Qing‐Yao Zhu

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China

X

Xiao‐Xue Wang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China

D

De‐Hui Guan

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China

J

Jian‐You Li

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China

X

Xin‐Yuan Yuan

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China

H

Huan‐Feng Wang

College of Materials and Chemical Engineering Zhengzhou Key Laboratory of Functional Electrocatalysis and Chemical Energy Storage Zhengzhou University of Technology Zhengzhou 450044 P.R. China

J

Ji‐Jing Xu

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P.R. China