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...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.展开更多
基金the National Key R&D Program of China(2021YFA1201503)National Natural Science Foundation of China(Nos.21972164,22279161,12264038,22309144)+7 种基金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 AssociationQ.Z.acknowledges the support of HZWTECH for providing computational facilitiesH.A.acknowledges the University of Hong Kong and the Hong Kong Quantum AI Lab Limited,AIR@Inno HK for supporting his fellowshipWe also thank Nano-X,Suzhou Institute of Nano-tech and Nano-bionics,Chinese Academy of Sciences for the material measurement analysisOpen Access funding enabled and organized by Projekt DEAL.
文摘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.
