Fast interfacial electrocatalytic desolvation enabling lowtemperature and long-cycle-life aqueous Zn batteries  

作　　者：Jian Wang Hongfei Hu Lujie Jia Jing Zhang Quan Zhuang Linge Li Yongzheng Zhang Dong Wang Qinghua Guan Huimin Hu Meinan Liu Liang Zhan Henry Adenusi Stefano Passerini Hongzhen Lin 

机构地区：[1]i-Lab&CAS Key Laboratory of Nanophotonic Materials and Devices,Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences,Suzhou,the People’s Republic of China [2]Helmholtz Institute Ulm(HIU),Ulm,Germany [3]Karlsruhe Institute of Technology(KIT),Karlsruhe,Germany [4]Inner Mongolia Key Laboratory of Carbon Nanomaterials,Nano Innovation Institute(NII),Inner Mongolia Minzu University,Tongliao,the People’s Republic of China [5]State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai,the People’s Republic of China [6]School of Materials Science&Engineering and International Center of Future Science,Jilin University,Changchun,Jilin,the People’s Republic of China [7]Department of Science and Engineering of Matter,Environment and Urban Planning,Marche Polytechnic University,Ancona,Italy [8]Department of Chemistry,The University of Hong Kong,Hong Kong,the People’s Republic of China [9]Hong Kong Quantum AI Lab,Hong Kong,the People’s Republic of China [10]Chemistry Department,Sapienza University of Rome,Rome,Italy

出　　处：《InfoMat》2024年第7期76-89,共14页信息材料（英文）

基　　金：the National Key R&D Program of China(2021YFA1201503);National Natural Science Foundation of China(Nos.21972164,22279161,12264038,22309144);the Natural Science Foundation of Jiangsu Province(BK.20210130);China Postdoctoral Science Foundation(2023 M732561,2023 M731084);Innovative and Entrepreneurial Doctor in Jiangsu Province(JSSCBS20211428);J.W.and S.P.acknowledge the funding provided by the Alexander von Humboldt Foundation and the basic funding of the Helmholtz Association;Q.Z.acknowledges the support of HZWTECH for providing computational facilities;H.A.acknowledges the University of Hong Kong and the Hong Kong Quantum AI Lab Limited,AIR@Inno HK for supporting his fellowship;We also thank Nano-X,Suzhou Institute of Nano-tech and Nano-bionics,Chinese Academy of Sciences for the material measurement analysis;Open Access funding enabled and organized by Projekt DEAL.

摘　　要：Low-temperature zinc batteries(LT-ZIBs)based on aqueous electrolytes show great promise for practical applications owing to their natural resource abundance and low cost.However,they suffer from sluggish kinetics with elevated energy barriers due to the dissociation of bulky Zn(H2O)62+solvation structure and free Zn2+diffusion,resulting in unsatisfactory lifespan and performance.Herein,dissimilar to solvation shell tuning or layer spacing enlargement engineering,delocalized electrons in cathode through constructing intrinsic defect engineering is proposed to achieve a rapid electrocatalytic desolvation to obtain free Zn2+for insertion/extraction.As revealed by density functional theory calculations and interfacial spectroscopic characterizations,the intrinsic delocalized electron distribution propels the Zn(H2O)62+dissociation,forming a reversible interphase and facilitating Zn2+diffusion across the electrolyte/cathode interface.The as-fabricated oxygen defect-rich V2O5 on hierarchical porous carbon(ODVO@HPC)electrode exhibits high capacity robustness from 25 to20℃.Operating at-20℃,the ODVO@HPC delivers 191 mAh g-1 at 50 A g-1 and lasts for 50000 cycles at 10 A g-1,significantly enhancing the power density and lifespan under low-temperature environments in comparison to previous reports.Even with areal mass loading of-13 mg cm2,both coin cells and pouch batteries maintain excellent stability and areal capacities,realizing practical high-performance LT-ZIBs.

关 键 词：defect catalysis delocalized electron engineering diffusion kinetics modulation lowtemperature Zn batteries V2O5 cathode 

分 类 号：TM912[电气工程—电力电子与电力传动]