机构地区:[1]College of Mechanical Engineering,Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials,Hunan Institute of Science and Technology,Yueyang 414006,Hunan,China [2]School of Materials Science and Engineering,Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province,Central South University,Changsha 410083,Hunan,China [3]College of Materials and Metallurgy,Guizhou University,Guiyang 550000,Guizhou,China [4]National Energy Metal Resources and New Materials Key Laboratory,Central South University,Changsha 410083,Hunan,China
出 处:《Journal of Energy Chemistry》2025年第1期684-692,共9页能源化学(英文版)
基 金:National Natural Science Foundation of China (52301273, 52072411);Science and Technology Innovation Program of Hunan Province (2024RC3222);Key project of scientific research project of Hunan Provincial Department of Education (22A0479);China Postdoctoral Science Foundation (2024M753668);Central South University Innovation-Driven Research Programme (2023CXQD038);Hunan Provincial Postgraduate Research Innovation Programme(CX20240970)。
摘 要:Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc (Zn) deposition and hydrogen evolution.Particularly,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn^(2+)-solvation and deposition behavior demand comprehensive investigation.Organic molecules endowed with special functional groups (such as hydroxyl,carboxyl,etc.) have the potential to significantly optimize the solvation structure of Zn^(2+)and regulate the interfacial electric double layer (EDL).By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn deposition.Herein,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn (H-Zn) anode with a uniform and dense structure.The interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare Zn.Consequently,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 h.Moreover,the H-Zn//NH_(4)V_(4)O^(10)(NVO) full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A g^(-1).This study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.
关 键 词:Aqueous zinc-ion batteries Zn^(2+)-solvation structure Interfacial reaction Asymptotic nucleation model Reversible and stable Zn anode
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