The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalyt...The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center.Therefore,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks.However,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application.Herein,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)ORR.Compared with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by 1000-fold.As a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction pathways.This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR.展开更多
A facile and efficient ball-milling assisted sol-gel synthesis route was developed to prepare triclinic e-LiVOPO_(4)(LVOP)material with lanthanum(La)and cerium(Ce)modification individually as well as simultaneously.An...A facile and efficient ball-milling assisted sol-gel synthesis route was developed to prepare triclinic e-LiVOPO_(4)(LVOP)material with lanthanum(La)and cerium(Ce)modification individually as well as simultaneously.An LVOP/LaPO_(4)/CePO_(4)composite cathode material was successfully synthesized and results show that La and Ce co-modification noticeably improves the electrochemical performance by enhancing the high voltage capacity upon cycling,which indicates contributions from the good ionic conductors LaPO_(4)and CePO_(4).The simultaneous La and Ce modification improves the high voltage performance significantly with an increase of 50%in high voltage capacity after 20 cycles compared to pure LVOP.It also shows stabilized cycling perfo rmance with 91%capacity rete ntion after 50 cycles at 0.1 C rate,along with high-rate capability with a capacity of 83.1 mAh/g compared to the pristine sample showing the capacity of 51.6 mAh/g at a high rate of 5C.This can be attributed to the good conductivity of LaPO_(4)and CePO_(4).In addition,the LVOP/LaPO_(4)/CePO_(4)composite and the pristine LVOP give a charge transfer resistance of-105 and-212Ω,respectively,showing much lower impedance due to a combination of La and Ce addition.展开更多
As an emerging member of the two-dimensional(2D)material family,V_(2)CT_(X)MXene shows great potential in the application of lithium-ion capacitors(LICs)due to its unique structure and excellent electrical conductivit...As an emerging member of the two-dimensional(2D)material family,V_(2)CT_(X)MXene shows great potential in the application of lithium-ion capacitors(LICs)due to its unique structure and excellent electrical conductivity.However,severe nanosheets stacking and intra-layer transport barriers have limited the further development of V_(2)CT_(X)MXene-based materials.Herein,we prepared Kions and–O functional group co-modified V_(2)CT_(X)MXene(VCT-K)and further incorporated it with single-walled carbon nanotube(SWCNT),obtaining freestanding V_(2)CT_(X)composite films(VCT-K@C)with the 3D conductive network.Significantly,K+ions were introduced into V_(2)CT_(X)MXene to stabilize the interlayer structure and prevent the aggregation of nanosheets,the terminal group of–O was controllably modified on the surface of MXene to improve the Li+ions storage reversible capacities and the SWCNT acted as the bridge between MXene nanosheets to opens up the channels for ion/electron transportation in the longitudinal direction.Benefited from the synergistic effect of VCT-K and SWCNT,the VCT-K@C exhibits superior reversible specific capacities of 671.8 mA h g^(-1)at 0.1 A g^(-1)and 318 mA h g^(-1)at 1.0 A g^(-1).Furthermore,the assembled LICs with VCT-K@C anode coupling activated carbon(AC)cathode deliver an outstanding power density of 19.0 kW kg^(-1)at 67.4 Wh kg^(-1),a high energy density of 140.5 Wh kg^(-1)at 94.8 W kg^(-1)and a stable capacitance retention of 86%after 6000 cycles at 10 A g^(-1).Such unique structures and excellent electrochemical properties are expected to pave the way for the large-scale application in LICs of MXene-based materials.展开更多
基金the financial support by the National Natural Science Foundation of China(Nos.22205124,52172206)Natural Science Foundation of Shandong province(Nos.ZR2021QB070,ZR2023QB110)+2 种基金Basic Research Projects for the Pilot Project of Integrating Science and Education and Industry of Qilu University of Technology(Shandong Academy of Sciences)(Nos.2023PY024,2023PX108)Special Fund for Taishan Scholars Projectthe Development Plan of Youth Innovation Team in Colleges and Universities of Shandong Province。
文摘The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center.Therefore,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks.However,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application.Herein,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)ORR.Compared with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by 1000-fold.As a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction pathways.This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR.
基金the Anhui Natural Science Foundation(1908085ME151,KJ2020A0263)China Po stdoctoral Science Foundation(2020M673404)+2 种基金Anhui Province High-end Talent Grant(DT18100044)the National Level Foreign Expert Introduction Plan(G20190219004)the National Natural Science Foundation of China(52207246)。
文摘A facile and efficient ball-milling assisted sol-gel synthesis route was developed to prepare triclinic e-LiVOPO_(4)(LVOP)material with lanthanum(La)and cerium(Ce)modification individually as well as simultaneously.An LVOP/LaPO_(4)/CePO_(4)composite cathode material was successfully synthesized and results show that La and Ce co-modification noticeably improves the electrochemical performance by enhancing the high voltage capacity upon cycling,which indicates contributions from the good ionic conductors LaPO_(4)and CePO_(4).The simultaneous La and Ce modification improves the high voltage performance significantly with an increase of 50%in high voltage capacity after 20 cycles compared to pure LVOP.It also shows stabilized cycling perfo rmance with 91%capacity rete ntion after 50 cycles at 0.1 C rate,along with high-rate capability with a capacity of 83.1 mAh/g compared to the pristine sample showing the capacity of 51.6 mAh/g at a high rate of 5C.This can be attributed to the good conductivity of LaPO_(4)and CePO_(4).In addition,the LVOP/LaPO_(4)/CePO_(4)composite and the pristine LVOP give a charge transfer resistance of-105 and-212Ω,respectively,showing much lower impedance due to a combination of La and Ce addition.
基金funded by the National Natural Science Foundation of China(Grant Nos.22005167 and 21905152)the Shandong Provincial Natural Science Foundation of China(Grant Nos.ZR2020QB125 and ZR2020MB045)+1 种基金the China Postdoctoral Science Foundation(Grant Nos.2021M693256,2021T140687 and 2022M713249)the Qingdao Postdoctoral Applied Research Project and the Youth Innovation Team Project for Talent Introduction and Cultivation in Universities of Shandong Province。
文摘As an emerging member of the two-dimensional(2D)material family,V_(2)CT_(X)MXene shows great potential in the application of lithium-ion capacitors(LICs)due to its unique structure and excellent electrical conductivity.However,severe nanosheets stacking and intra-layer transport barriers have limited the further development of V_(2)CT_(X)MXene-based materials.Herein,we prepared Kions and–O functional group co-modified V_(2)CT_(X)MXene(VCT-K)and further incorporated it with single-walled carbon nanotube(SWCNT),obtaining freestanding V_(2)CT_(X)composite films(VCT-K@C)with the 3D conductive network.Significantly,K+ions were introduced into V_(2)CT_(X)MXene to stabilize the interlayer structure and prevent the aggregation of nanosheets,the terminal group of–O was controllably modified on the surface of MXene to improve the Li+ions storage reversible capacities and the SWCNT acted as the bridge between MXene nanosheets to opens up the channels for ion/electron transportation in the longitudinal direction.Benefited from the synergistic effect of VCT-K and SWCNT,the VCT-K@C exhibits superior reversible specific capacities of 671.8 mA h g^(-1)at 0.1 A g^(-1)and 318 mA h g^(-1)at 1.0 A g^(-1).Furthermore,the assembled LICs with VCT-K@C anode coupling activated carbon(AC)cathode deliver an outstanding power density of 19.0 kW kg^(-1)at 67.4 Wh kg^(-1),a high energy density of 140.5 Wh kg^(-1)at 94.8 W kg^(-1)and a stable capacitance retention of 86%after 6000 cycles at 10 A g^(-1).Such unique structures and excellent electrochemical properties are expected to pave the way for the large-scale application in LICs of MXene-based materials.
