Crystal Transformation Strategy in Hydrogen‐Bonded Organic Framework Solid‐State Electrolyte for Stable Zinc‐Ion Batteries

J Jia‐Xin Li (State Key Laboratory of Medical Chemical Biology College of Pharmacy Nankai University Tianjin People's Republic of 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) D De‐Hui Guan (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) C Cheng‐Lin Miao (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 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 zinc ion batteries (ZIBs) hold great potential for sustainable and high‐safety reserves. However, the advancement of solid‐state ZIBs is constrained by the shortage of reasonable solid‐state electrolytes (SSE) with abundant hopping sites, effective hydrogen evolution reaction (HER) inhibition, and favorable interfacial compatibility. Herein, the hydrogen‐bonded organic framework (HOF) CAM‐Ag with Zn 2+ hopping sites is developed as SSE for ZIBs. Taking advantage of the short‐distance Zn 2+ conduction pathways by crystal transformation through incorporating the Ag−N coordinate bonds, CAM‐Ag SSE achieves a significant ionic conductivity of 1.14 × 10 −4  S cm −1 at room temperature and superior Zn 2+ transference number of 0.72. An abundant hydrogen bonds network effectively inhibits the initiation of HER and the subsequent generation of by‐products. Moreover, the rapid Zn 2+ conduction kinetics facilitated the inhibition of dendrite growth, promoting the uniform Zn 2+ distribution. CAM‐Ag SSE displays an extensive electrochemical stability range of 0–2.66 V and remarkable electrochemical compatibility, enabling stable Zn 2+ plating/stripping for ≈1000 h at 1 mA cm −2 . Consequently, CAM‐Ag SSE‐based solid‐state ZIBs achieve a specific capacity of 315 mAh g −1 with only 1.5% decrease in capacitance after 24 h. The proposed HOF‐based SSE displays a potential pathway for advancing stable and high‐performance solid‐state ZIBs.

Article Details

Volume / Issue Vol. 37, Issue 34
Published August 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (6)

J

Jia‐Xin Li

State Key Laboratory of Medical Chemical Biology College of Pharmacy Nankai University Tianjin People's Republic of 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

D

De‐Hui Guan

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

C

Cheng‐Lin Miao

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 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