The practical deployment of aqueous zinc metal batteries(AZMBs)is critically challenged by uncontrolled dendrite formation and parasitic side reactions,both arising from unstable interfacial chemistry.Herein,we propos...The practical deployment of aqueous zinc metal batteries(AZMBs)is critically challenged by uncontrolled dendrite formation and parasitic side reactions,both arising from unstable interfacial chemistry.Herein,we propose a dual-region interfacial engineering strategy that concurrently regulates both the outer and inner Helmholtz planes(OHP/IHP)by introducing the N,N-dimethylethanolamine(DMEA)into the ZnSO_(4) electrolyte.In the OHP,DMEA coordinates with Zn^(2+)to reshape the solvation structure and attenuate Zn^(2+)-H_(2)O interactions,thereby lowering water activity and suppressing hydrogen evolution.Meanwhile,DMEA molecules chemisorb onto the Zn surface within the IHP,forming a robust organic interphase that homogenizes the electric field and promotes uniform Zn nucleation.This dual functionality guides crystallographic evolution toward the thermodynamically favorable(101)facet,which supports lateral Zn growth and effectively mitigates dendrite propagation.Benefiting from the interfacial-crystallographic synergy,Zn‖Zn symmetric cells exhibit ultralong cycling stability over5000 h at 1 mA cm^(-2) and maintain dendrite-free operation for over 1000 h at 5 mA cm^(-2).Furthermore,Zn‖NH_(4)V_(4)O_(10) full cells deliver high specific capacities with 80.06%capacity retention after1000 cycles at 5 A g^(-1).This work offers a mechanistically guided and scalable electrolyte design that bridges solvation chemistry with crystallographic control,providing a promising route toward dendrite-free,high-efficiency AZMBs.展开更多
基金the financial support from the Scientific Research Fund of Liaoning Provincial Education Department of China(No.JYTQN2023289)the Liaoning Provincial Science and Technology Joint Plan(Fund)Project(No.2023BSBA-259)+4 种基金the opening project of State Key Laboratory of Metastable Materials Science and Technology,Yanshan University(No.202404)the support from the National Natural Science Foundation of China(Grant No.52402279)the China Postdoctoral Science Foundation Special Funding(Grant No.T2025T180002)the China Postdoctoral Science Foundation General Program(Grant No.2024M751753)the opening project of State Key Laboratory of Metastable Materials Science and Technology(Yanshan University)(No.202401)。
文摘The practical deployment of aqueous zinc metal batteries(AZMBs)is critically challenged by uncontrolled dendrite formation and parasitic side reactions,both arising from unstable interfacial chemistry.Herein,we propose a dual-region interfacial engineering strategy that concurrently regulates both the outer and inner Helmholtz planes(OHP/IHP)by introducing the N,N-dimethylethanolamine(DMEA)into the ZnSO_(4) electrolyte.In the OHP,DMEA coordinates with Zn^(2+)to reshape the solvation structure and attenuate Zn^(2+)-H_(2)O interactions,thereby lowering water activity and suppressing hydrogen evolution.Meanwhile,DMEA molecules chemisorb onto the Zn surface within the IHP,forming a robust organic interphase that homogenizes the electric field and promotes uniform Zn nucleation.This dual functionality guides crystallographic evolution toward the thermodynamically favorable(101)facet,which supports lateral Zn growth and effectively mitigates dendrite propagation.Benefiting from the interfacial-crystallographic synergy,Zn‖Zn symmetric cells exhibit ultralong cycling stability over5000 h at 1 mA cm^(-2) and maintain dendrite-free operation for over 1000 h at 5 mA cm^(-2).Furthermore,Zn‖NH_(4)V_(4)O_(10) full cells deliver high specific capacities with 80.06%capacity retention after1000 cycles at 5 A g^(-1).This work offers a mechanistically guided and scalable electrolyte design that bridges solvation chemistry with crystallographic control,providing a promising route toward dendrite-free,high-efficiency AZMBs.
