Ni‐Bis(dithiolene) Coordination Enhanced Dual‐Functional Covalent Organic Frameworks for both Cathodic Zn <sup>2+</sup> Storage and Anodic Zinc Deposition Control in Aqueous Zn‐Ion Batteries

Q Qianchuan Yu (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering) T Tianyu Shen (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering) S Si‐Wen Ke (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, School of Sustainable Energy and...) K Kaiqiang Zhang X Xinmei Song (Key Laboratory of Luminescence Analysis and Molecular Sensing, Ministry of Education, School of Chemistry and Chemical Engineering) J Jingjie Sun Z Zuoao Wu (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Sustainable Energy and Resources, School of Chemistry and Chemical Engineering) M Miao Wang Y Yongxin Yang Z Zedong Zhang (School of Materials Science and Engineering) A Anqi Zhang Z Zuoxiu Tie (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Green Energy Catalysis and Intelligent Chemical Engineering, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering) Y Yichao Yan (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Sustainable Energy and Resources, School of Chemistry and Chemical Engineering) J Jing Ma (State Key Laboratory of Coordination Chemistry, School of Chemistry) J Jinglin Zuo (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, School of Sustainable Energy and...) Z Zhong Jin (State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Green Energy Catalysis and Intelligent Chemical Engineering, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering)

Abstract

Abstract In response to the increasing demand for sustainable energy storage solutions, aqueous zinc‐ion batteries (AZIBs) have garnered significant attention for their high safety, low cost, and environmental friendliness. However, two major challenges to battery stability persist: developing efficient cathode materials and addressing zinc dendrite formation. Here, we report a dual‐functional covalent organic framework (COF), named Ni–DAPTO, designed to improve both Zn 2+ storage on the cathode and zinc deposition kinetics on the anode. The incorporation of Ni coordination centers achieves an expected low energy gap, enhancing the intrinsic conductivity, while selectively guiding uniform Zn 2+ deposition. As a result, the Ni–DAPTO cathode demonstrated superior cycling stability and rate performance, retaining a specific capacity of 127.0 and 119.7 mAh g −1 at 0.5 and 10.0 A g −1 , respectively after 10 000 cycles. Besides, when employed as artificial solid electrolyte interphase (SEI), Ni–DAPTO can improve zinc utilization and inhibit dendrite formation. The full AZIBs assembled with Ni–DAPTO cathodes and Ni–DAPTO modified Zn anodes deliver a discharge capacity of 100.9 mAh g −1 after 1000 cycles at a current density of 5.0 A g −1 . These findings suggest that multifunctional COFs hold great potential for advancing high‐performance and long‐lasting aqueous secondary batteries.

Article Details

Volume / Issue Vol. 64, Issue 37
Published September 08, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (16)

Q

Qianchuan Yu

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering

T

Tianyu Shen

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering

S

Si‐Wen Ke

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, School of Sustainable Energy and...

K

Kaiqiang Zhang

X

Xinmei Song

Key Laboratory of Luminescence Analysis and Molecular Sensing, Ministry of Education, School of Chemistry and Chemical Engineering

J

Jingjie Sun

Z

Zuoao Wu

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Sustainable Energy and Resources, School of Chemistry and Chemical Engineering

M

Miao Wang

Y

Yongxin Yang

Z

Zedong Zhang

School of Materials Science and Engineering

A

Anqi Zhang

Z

Zuoxiu Tie

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Green Energy Catalysis and Intelligent Chemical Engineering, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering

Y

Yichao Yan

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Sustainable Energy and Resources, School of Chemistry and Chemical Engineering

J

Jing Ma

State Key Laboratory of Coordination Chemistry, School of Chemistry

J

Jinglin Zuo

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, School of Sustainable Energy and...

Z

Zhong Jin

State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Green Energy Catalysis and Intelligent Chemical Engineering, Suzhou Key Laboratory of Green Intelligent Manufacturing of New Energy Materials and Devices, Tianchang New Materials and Energy Technologies Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering