Diffusionless-Like Transformation Unlocks Pseudocapacitance with Bulk Utilization:Reinventing Fe2O3 in Alkaline Electrolyte

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外文摘要：Energy density can be substantially raised and even maximized if the bulk of an electrode material is fully utilized.Transition metal oxides based on conversion reaction mechanism are the imperative choice due to either constructing nanostructure or intercalation pseudocapacitance with their intrinsic limitations.However,the fully bulk utilization of transition metal oxides is hindered by the poor understanding of atomic-level conversion reaction mechanism,particularly it is largely missing at clarifying how the phase transformation(conversion reaction)determines the electrochemical performance such as power density and cyclic stability.Herein,α-Fe2O3 is a case provided to claim how the diffusional and diffusionless transformation determine the electrochemical behaviors,as of its conversion reaction mechanism with fully bulk utilization in alkaline electrolyte.Specifically,the discharge product α-FeOOH diffusional from Fe(OH)2 is structurally identified as the atomic-level arch criminal for its cyclic stability deterioration,whereas the counterpart δ-FeOOH is theoretically diffusionless-like,unlocking the full potential of the pseudocapacitance with fully bulk utilization.Thus,such pseudocapacitance,in proof-of-concept and termed as conversion pseudocapacitance,is achieved via diffusionless-like transformation.This work not only provides an atomic-level perspective to reassess the potential electrochemical performance of the transition metal oxides electrode materials based on conversion reaction mechanism but also debuts a new paradigm for pseudocapacitance.

外文关键词：

bulk utilizationconversion pseudocapacitancediffusion less transformationFe2O33phase transformation

作者：

Taowen Dong、Wencai Yi、Ting Deng、Tingting Qin、Xianyu Chu、He Yang、Lirong Zheng、Seung Jo Yoo、Jin-Gyu Kim、Zizhun Wang、Yan Wang、Wei Zhang、Weitao Zheng

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作者单位：

State Key Laboratory of Automotive Simulation and Control,and School of Materials Science & Engineering,Key Laboratory of Automobile Materials MOE,and Electron Microscopy Center,and International Center of Future Science,Jilin University,Changchun 130012,China

Laboratory of High Pressure Physics and Material Science(HPPMS),School of Physics and Physical Engineering,Qufu Normal University,Qufu 273165,China

Beijing Synchrotron Radiation Facility,Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China

Electron Microscopy Research Center,Korea Basic Science Institute,Daejeon 34133,South Korea

Wuhan National Laboratory for Optoelectronics,Huazhong University of Science and Technology,Wuhan 430074,China

IKERBASQUE,Basque Foundation for Science,Bilbao 48013,Spain

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基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of China2020 International Cooperation Project of the Department of Science and Technology of Jilin ProvinceProgram for the Development of Science and Technology of Jilin ProvinceJilin Province/Jilin University Co-Construction Project-Funds for New MaterialsJilin Province/Jilin University Co-Construction Project-Funds for New MaterialsProject for Selfinnovation Capability Construction of Jilin Province Development and Reform CommissionOpen Project Program of Wuhan National Laboratory for OptoelectronicsProgram for J LU Science and Technology Innovative Research TeamProgram for J LU Science and Technology Innovative Research Team

项目编号：

519320035187211520200801001GH20190201309JCSXGJSF2017-3Branch-2/440050316A362021C0262018WNLOKF022JLUSTIRT2017TD-09

出版年：

2023

DOI：

10.1002/eem2.12262

能源与环境材料(英文)

CSCD

ISSN：

年,卷(期)：2023.6(1)

参考文献量59