Ultrathin Mesoporous Ionic Brushes Separator Enables Fast and Durable Zinc‐Metal Aqueous Batteries
Abstract
ABSTRACT Zinc metal aqueous batteries (ZnABs) emerge as promising candidates for grid‐scale energy storage, yet severe Zn dendrite formation and anode side reactions degrade cycle life and hinder practical application. Herein, we report an ultrathin (27 µm) mesoporous ionic brushes (MiB) separator based on sulfonic grafted ordered mesoporous silica nanosheets for stable ZnABs. The well‐ordered perforative mesopores architecture functions as an ion rectifier that achieves enhanced transfer kinetics and a homogeneous concentration field, thereby promoting dendrite‐free deposition, as verified by in situ digital holography and kinetic analyses. Moreover, ionic brushes confined within nanochannels selectively capture water molecules from the primary solvation shell of Zn 2+ , facilitating desolvation and constructing a localized water‐lean interfacial environment, which effectively suppresses water‐related side reactions, as evidenced by various in situ spectroscopy, electrochemical analyses, and theoretical calculations. Consequently, the MiB separator enables the Zn anode to achieve a high Coulombic efficiency of 99.7%, ultralong lifespan over 4300 h, fast plating kinetics of 20 mA cm −2 , and high Zn utilization rate of 51.6%. Furthermore, Zn‐V 2 O 5 cells achieve perdurable capacity retention of 91.5% after 3500 cycles. This work presents a rational mesoporous separator design that synchronously regulates ion transport and interfacial solvation chemistry for highly reversible ZnABs.
Article Details
Authors (17)
Yucai Wu
Department of Chemistry Laboratory of Advanced Materials Aqueous Battery Center Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Shanghai Wusong Laboratory of Materials Science Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Porous Materials for Separation and Conversion College of Smart Materials and Future Energy Fudan University Shanghai China
Wanhai Zhou
Laboratory of Advanced Materials, Aqueous Battery Center, College of Smart Materials and Future Energy
Hongrun Jin
Gaoyang Li
Xia Wang
Lipeng Wang
College of Chemistry and Materials, Department of Chemistry, Laboratory of Advanced Materials
Huan Du
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering
Zhihao Sun
Rice Research Institute, Key Laboratory of Crop Molecular Improvement, Academy of Agricultural Sciences, Southwest University
Shixiang Ding
Tengsheng Zhang
Laboratory of Advanced Materials, Aqueous Battery Center, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Electron Microscope Center of Fudan University, Shanghai Wusong Laboratory of Materials Science, and Faculty of Chemistry and Materials
Junwei Zhang
Fanxing Bu
Zaiwang Zhao
College of Energy Materials and Chemistry, College of Chemistry and Chemical Engineering
Chao Ye
School of Chemical Engineering
Wei Li
Dongliang Chao
Laboratory of Advanced Materials, Aqueous Battery Center, College of Smart Materials and Future Energy
Dongyuan Zhao
Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, State Key Laboratory of Porous Materials for Separation and Conversion, Fudan University, 220 Handan, Shanghai 200433, P. R. China