Efficient energy storage devices,i.e.pseudocapacitors,are being intensively pursued to address the environmental and energy crises.Most high-performance pseudocapacitors are based on inorganic materials,while organic ...Efficient energy storage devices,i.e.pseudocapacitors,are being intensively pursued to address the environmental and energy crises.Most high-performance pseudocapacitors are based on inorganic materials,while organic materials with broader synthetic tunability have attracted increasing interest.Despite recent progress,electron-deficient(n-type)organic pseudocapacitive materials for flexible energy storage are highly demanded yet remain largely unexplored.Here a novel set of n-type perylene diimide(PDI)based conjugated microporous polymers(CMPs),namely,CMP-1,CMP-2 and CMP-3,have been created to integrate excellent desirable characteristics as organic pseudocapacitor electrode materials for flexible energy storage.In light of electron-accepting redox-active sites,hierarchically porous structures,as well as amide-linked networks,the PDI-CMPs electrodes displayed n-type pseudocapacitive behaviors with high capacity(139-205 F g^(-1)at 0.5 A g^(-1)),wide and negative biases(-1.0 to 0 V vs.Ag/AgCl),and long cycling stability.CMP-3 consisting of tetraphenylmethane three-dimensional(3D)building block and PDI units demonstrates not only higher capacitance but also better performance stability because of the higher specific surface area and faster diffusion kinetics as compared to its counterpart CMP-1.Asymmetric supercapacitors(SCs)based on CMP-3 and poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)(PEDOT/PSS)exhibited wider potential window(1.8 V)and higher capacitance(17.4 m F cm^(-2))compared with symmetric SCs based on PEDOT/PSS electrodes.Notably,CMP-3 also demonstrates attractive potentials as the anode for rechargeable Li-ion batteries.The study sheds light on the fundamental understanding of the key structural parameters that determine their electrochemical and transport properties,thus opening a new door for the rational design of efficient and stable n-type organic electrode materials for flexible energy storage applications.展开更多
基金supported by the National Natural Science Foundation of China(21835003,91833304,21422402,21604043,21674050,and 62004106)the National Key Basic Research Program of China(973 Program,2014CB648300 and 2017YFB0404501)+10 种基金the Natural Science Foundation of Jiangsu Province(BK20160888 and BE2019120)the Program for Jiangsu Specially-Appointed Professor(RK030STP15001)the Six Talent Peaks Project of Jiangsu Province(TD-XCL-009)the 333 Project of Jiangsu Province(BRA2017402)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(20KJB140005)China Postdoctoral Science Foundation(2020M671553)the NUPT“1311 Project”Scientific Foundation(NY217169,NY215062,NY215107,and NY217087)the Leading Talent of Technological Innovation of National Ten-Thousands Talents Program of China,the Excellent Scientific and Technological Innovative Teams of Jiangsu Higher Education Institutions(TJ217038)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(SJCX21-0297)the Synergetic Innovation Center for Organic Electronics and Information Displays,and the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
基金supported by the National Natural Science Foundation of China(21835003,62004106,21422402,21674050,61904084)the Natural Science Foundation of Jiangsu Province(BE2019120,BK20190737,BK20210601 and BK20190737)+10 种基金the National Key Basic Research Program of China(2014CB648300,2017YFB0404501)China Postdoctoral Science Foundation(2020M671553 and 2021M691652)Program for Jiangsu Specially-Appointed Professor(RK030STP15001)the Six Talent Peaks Project of Jiangsu Province(TDXCL-009)the 333 Project of Jiangsu Province(BRA2017402)the NUPT“1311 Project”Scientific Foundation(NY217169,NY215062,NY217087)the Leading Talent of Technological Innovation of National Ten-Thousands Talents Program of Chinathe Excellent Scientific and Technological Innovative Teams of Jiangsu Higher Education Institutions(TJ217038)the Synergetic Innovation Center for Organic Electronics and Information Displaysthe Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Efficient energy storage devices,i.e.pseudocapacitors,are being intensively pursued to address the environmental and energy crises.Most high-performance pseudocapacitors are based on inorganic materials,while organic materials with broader synthetic tunability have attracted increasing interest.Despite recent progress,electron-deficient(n-type)organic pseudocapacitive materials for flexible energy storage are highly demanded yet remain largely unexplored.Here a novel set of n-type perylene diimide(PDI)based conjugated microporous polymers(CMPs),namely,CMP-1,CMP-2 and CMP-3,have been created to integrate excellent desirable characteristics as organic pseudocapacitor electrode materials for flexible energy storage.In light of electron-accepting redox-active sites,hierarchically porous structures,as well as amide-linked networks,the PDI-CMPs electrodes displayed n-type pseudocapacitive behaviors with high capacity(139-205 F g^(-1)at 0.5 A g^(-1)),wide and negative biases(-1.0 to 0 V vs.Ag/AgCl),and long cycling stability.CMP-3 consisting of tetraphenylmethane three-dimensional(3D)building block and PDI units demonstrates not only higher capacitance but also better performance stability because of the higher specific surface area and faster diffusion kinetics as compared to its counterpart CMP-1.Asymmetric supercapacitors(SCs)based on CMP-3 and poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)(PEDOT/PSS)exhibited wider potential window(1.8 V)and higher capacitance(17.4 m F cm^(-2))compared with symmetric SCs based on PEDOT/PSS electrodes.Notably,CMP-3 also demonstrates attractive potentials as the anode for rechargeable Li-ion batteries.The study sheds light on the fundamental understanding of the key structural parameters that determine their electrochemical and transport properties,thus opening a new door for the rational design of efficient and stable n-type organic electrode materials for flexible energy storage applications.
