Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challeng...Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.展开更多
Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by t...Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.展开更多
基金supported by the “Pioneer” and “Leading Goose” R&D Program of Zhejiang Province of China (No. 2024C01056)the support from London South Bank University
文摘Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.
基金supported by the National Natural Science Foundation of China(No.22109181,U24A2060,22279023,and 22309031)the National Key R&D Program of China(2024YFE0101100)+6 种基金the Hunan Provincial Science and Technology Plan Projects of China(No.2017TP1001)the Hunan Provincial Natural Science Foundation of China(No.2025JJ40011)the Fundamental Research Funds for the Central Universities(20720250005)the Science and Technology Commission of Shanghai Municipality(25DZ3002901,2024ZDSYS02,25PY2600100)the Shanghai Pilot Program for Basic Research-Fudan University 21TQ1400100(25TQ012)the AI for Science Foundation of Fudan University(FudanX24A1035)the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.
