文献类型：期刊文献

英文题名：Non-Covalent Molecular Engineering of Hydrogel Electrolytes via π-Anion Confinement and Hydrogen-Bond Reconfiguration for Wide-Temperature and Ultra-Stable Zn-Ion Batteries

作者：Zhong, Jia[1]; Xia, Chuqiao[1]; Zhang, Tianyu[2]; Wang, Hongfei[1]; Tao, Haolan[3]; Lian, Cheng[3]; Hu, Yong[2]

机构：[1] Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Department of Chemistry, Zhejiang Normal University, Jinhua, 321004, China; [2] Institute of Nanocatalysis and Energy Conversion, College of Chemistry and Materials Engineering, Zhejiang A&F University, Hangzhou, 311300, China; [3] State Key Laboratory of Chemical Engineering, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China

年份：2025

外文期刊名：Advanced Functional Materials

收录：EI(收录号：20254919627679)

语种：英文

外文关键词：Amides - Negative ions - Thermal Engineering - Vanadium compounds - Zinc - Zinc compounds

摘要：The practical application of Zn-ion batteries (ZIBs) is hindered by poor cycling stability and a narrow operating temperature window, issues stemming from the unstable Zn anode and the reactive nature of aqueous electrolyte. To overcome these challenges, a functional hydrogel electrolyte is developed via copolymerization of acrylamide (AM) and 2-phenoxyethyl acrylate (PHEA). This design utilizes a novel non-covalent molecular engineering strategy to simultaneously regulate Zn2+ transport and enhance thermal adaptability. Specifically, the electron-deficient phenyl rings in PHEA establish favorable π-anion interactions with OTf– anions, achieving a high Zn2+ transference number of 0.70. Concurrently, spectroscopic analyses indicate that the oxygen-rich groups in PHEA act as competitive hydrogen-bond acceptors, reconstructing the hydrogel's hydrogen-bonding network. This reconfiguration leads to tighter confinement of water molecules and a broader operational temperature range. Consequently, Zn//Zn symmetric cells demonstrate exceptional cycling durability over 6400 h at 25°C, 2400 h at 50°C, and 1200 h at –20°C. When paired with Zn2V2O7 cathodes, full cells also deliver outstanding cycling performance and remarkable capacity retention across this wide temperature range. This work provides fundamental insights into non-covalent interactions for electrolyte design and presents a scalable strategy for developing robust, temperature-resilient energy storage. ? 2025 Wiley-VCH GmbH.