journal article·2024-05Open access

Molecular Engineering Enables Hydrogel Electrolyte with Ionic Hopping Migration and Self‐Healability toward Dendrite‐Free Zinc‐Metal Anodes

Kaiping Zhu, Jie Luo, Dehe Zhang, Nanyang Wang, Shibo Pan, Shujin Zhou, Zhenjie Zhang, Gengde Guo, Peng Yang, Yuan Fan, Shisheng Hou, Zhipeng Shao, Shizhuo Liu, Lin Lin, Pan Xue, Guo Hong, Yurong Yang, Yagang Yao

Advanced Materials· Volume 36· Issue 19

Abstract

Abstract Hydrogel electrolytes (HEs), characterized by intrinsic safety, mechanical stability, and biocompatibility, can promote the development of flexible aqueous zinc‐ion batteries (FAZIBs). However, current FAZIB technology is severely restricted by the uncontrollable dendrite growth arising from undesirable reactions between the HEs with sluggish ionic conductivity and Zn metal. To overcome this challenge, this work proposes a molecular engineering strategy, which involves the introduction of oxygen‐rich poly(urea‐urethane) (OR‐PUU) into polyacrylamide (PAM)‐based HEs. The OR‐PUU/PAM HEs facilitate rapid ion transfer through their ionic hopping migration mechanism, resulting in uniform and orderly Zn2+ deposition. The abundant polar groups on the OR‐PUU molecules in OR‐PUU/PAM HEs break the inherent H‐bond network, tune the solvation structure of hydrated Zn2+, and inhibit the occurrence of side reactions. Moreover, the interaction of hierarchical H‐bonds in the OR‐PUU/PAM HEs endows them with self‐healability, enabling in situ repair of cracks induced by plating/stripping. Consequently, Zn symmetric cells incorporating the novel OR‐PUU/PAM HEs exhibit a long cycling life of 2000 h. The resulting Zn–MnO2 battery displays a low capacity decay rate of 0.009% over 2000 cycles at 2000 mA g−1. Overall, this work provides valuable insights to facilitate the realization of dendrite‐free Zn‐metal anodes through the molecular engineering of HEs.
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Research context

OpenAlex topics: Advanced battery technologies research · Advanced Battery Materials and Technologies · Perovskite Materials and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

National Laboratory of Solid State Microstructures College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China

Key Laboratory of Multifunctional Nanomaterials and Smart Systems Suzhou Institute of Nano‐Tech and Nano‐Bionics Chinese Academy of Sciences Suzhou 215123 China

Faculty of Physics Central South University Changsha 410083 P. R. China

Key Laboratory of Mesoscopic Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing 210093 China

Center of Energy Storage Materials & Technology College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials National Laboratory of Solid State Microstructures, and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210023 China

School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 China

Department of Materials Science and Engineering & Center of Super‐Diamond and Advanced Films City University of Hong Kong 83 Tat Chee Avenue Kowloon Hong Kong SAR 999077 China

Funding

National Key Research and Development Program of China · Natural Science Foundation of Jiangsu Province

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