Molecular Design of Polymeric Metal–Organic Nanocapsule Networks for Solid‐State Lithium Batteries

X Xin‐Yue Ma (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) C Cheng‐Lin Miao (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) Q Qing‐Yao Zhu (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 electrolytes (SSEs) have emerged as high‐priority materials for ensuring the safe operation of solid‐state lithium (Li) batteries. However, current SSEs still face challenges of balancing stability and ionic conductivity, which limits their practical applications in solid‐state Li batteries. Here, we report a general strategy for achieving high‐performance SSEs by constructing a Li + ‐conducted polymeric metal–organic nanocapsule (PolyMONC(Li)) network through molecular design. With the unique cage structure and pore size, metal–organic nanocapsule (MONC) can achieve excellent anion confinement effects. The PolyMONC(Li) network with continuous Li + conduction pathways serves as a solid electrolyte exhibiting a high ionic conductivity (0.18 mS cm −1 at 25 °C) and a high Li + transference number (0.83). Combining the two superiorities of optimal balance between mechanical strength and excellent Li + conductivity, the PolyMONC(Li) can still restrain the dendrite growth and prevent Li symmetric batteries from short‐circuiting even over 900 h cycling. The PolyMONC(Li)‐based SSEs Li‐metal batteries achieved a higher specific capacity than common polymer electrolytes such as polyethylene oxide‐based SSE. Additionally, taking advantage of the PolyMONC(Li) electrode binder, the solid‐state Li–O 2 battery achieves a stable cycling over 400 cycles. This work provides a comprehensive guideline for developing porous solids from molecule design to practical application.

Article Details

Volume / Issue Vol. 64, Issue 29
Published July 14, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (7)

X

Xin‐Yue Ma

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

C

Cheng‐Lin Miao

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

Q

Qing‐Yao Zhu

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