Single-Molecule Confinement Induced Intrinsic Multi-Electron Redox-Activity to Enhance Supercapacitor Performance

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外文摘要：Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage systems.To address this challenge,here,the precise confinement of single Keggin-type POM molecule in a porous carbon(PC)of unimodal super-micropore(micro-PC)is realized.Such precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM,which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron redox-activity.In particular,the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical calculation.Meanwhile,the molecularly dispersed POM molecules confined steadily in the"cage"of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of～11.4 wt％.As a result,the fabricated solid-state supercapacitor achieves a remarkable areal capacitance,ultrahigh energy and power density of 443 mF cm-2,0.12 mWh cm-2 and 21.1 mW cm-2,respectively.This work establishes a novel strategy for the precise confinement of single POM molecule,providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.

外文关键词：

intrinsic redox-activitypolyoxometalatessingle-molecule confinementsupercapacitor

作者：

Su Yang、Meiling Wang、Yong Zhang、Pinyi He、Wenhua Cong、Chongji Wang、Qiankun Yang、Xuguang Liu、Tian Wang、Xianming Zhang、Jiadong Zhou

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作者单位：

College of Materials Science and Engineering,Taiyuan University of Technology,Taiyuan 030024,China

Key Lab of Advanced Optoelectronic Quantum Architecture and Measurement(Ministry of Education),Beijing Key Lab of Nanophotonics &Ultrafine Optoelectronic Systems,and School of Physics,Beijing Institute of Technology,Beijing 100081,China

School of Materials Science and engineering,Central South University,Changsha 410083,China

Department of Chemistry,National University of Singapore,3 Science Drive 3,117543,Singapore

Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education,(Taiyuan University of Technology),Taiyuan 030024,China

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基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of China

项目编号：

51902222519722262174013

出版年：

2023

DOI：

10.1002/eem2.12396

能源与环境材料(英文)

CSCD

ISSN：

年,卷(期)：2023.6(4)

参考文献量62