The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(P...The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.展开更多
The growth kinetics of spherical NiAl and CuZr crystals are studied by using molecular dynamics simulations. The growth rates of crystals are found to increase with the grain radius. The simulations show that the inte...The growth kinetics of spherical NiAl and CuZr crystals are studied by using molecular dynamics simulations. The growth rates of crystals are found to increase with the grain radius. The simulations show that the interface thickness and the Jackson α-faetor increase as the growth proceeds, indicating that the interface becomes increasingly rough during growth. Due to the increasing interface roughening, the fraction of repeatable growth sites at interface f is proposed to actually increase in growth. An attachment rate, which is defined as the fraction of atoms that join the crystal interface without leaving, is used to approximate f, displaying a linear increase. With this approximation, we predict the growth rates as a function of the crystal radius, and the results qualitatively agree with those from the direct simulations.展开更多
Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity...Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.展开更多
Carbon cloth(CC)-based electrodes have attracted extensive attention for next-generation wearable energy-storage devices due to their excellent electrical conductivity and mechanical flexibility.However,the applicatio...Carbon cloth(CC)-based electrodes have attracted extensive attention for next-generation wearable energy-storage devices due to their excellent electrical conductivity and mechanical flexibility.However,the application of conventional CC-based electrodes for zinc(Zn)storage severely hinders Zn ion transport and induces deleterious Zn dendrite growth,resulting in poor electrochemical reliability.Herein,a novel oxygen plasma-treated carbon cloth(OPCC)is rationally designed as a current collector for flexible hybrid Zn ion supercapacitors(ZISs).The modified interface of OPCC with abundant oxygenated groups enables enhanced electrolyte wettability and uniform superficial electric field distribution.A prolonged working lifespan for Zn electrodeposition is achieved by the OPCC due to the improved interfacial kinetics and homogenized ion gradient.The as-prepared hybrid ZIS also delivers excellent cycling endurance(98.5%capacity retention for 1500 cycles)with outstanding operation stability under various extreme conditions.This facile surface modification strategy provides a new way for developing future flexible electrodes for wearable electronic products.展开更多
To conquer severe dendrites formation and side reactions of zinc metal anodes,which are serious obstacles for the practical applications of aqueous zinc ion battery(ZIB),herein,we develop a sodium allysulfonate(SAS)an...To conquer severe dendrites formation and side reactions of zinc metal anodes,which are serious obstacles for the practical applications of aqueous zinc ion battery(ZIB),herein,we develop a sodium allysulfonate(SAS)and acrylamide(AM)copolymer by radical polymerization process(crosslinking of C=C)as solid-state electrolyte.The interface kinetics is improved remarkably due to the high adhesion and excellent ion transferability of AM-SAS(AS)copolymers.Especially the sulfonic acid group in the hydrogel electrolyte can enhance the internal ionic conductivity effectively benefiting from its high affinity to Zn^(2+).Also,polymer chains realize re-regulation to Zn^(2+)flow in atomic-scale,thus leading to controllable deposition of Zn onto the dendrite-free Zn anodes.Consequently,the AS-1.5 electrolyte achieves ultra-stable Zn deposition/stripping behaviors with the lifespan over 1,000 h via the suppression of side-reactions and paralleled Zn deposition.High performances of Zn/Mn-doped V_(2)O_(5)(MnVO)(over 500 cycles)and Zn/diquinoxalino[2,3-a:2',3'-c]phenazine(HATN)(over 2,500 cycles)full cells demonstrate that the AS hydrogel electrolyte is a common approach for ZIBs under various conditions.This molecular regulation engineering opens a novel route for hydrogel electrolyte fabrication,where sulfonic groups perform as media of Zn^(2+)transfer.Therefore,high bulk ionic conductivity as well as excellent interface ion diffusion ability is obtained.展开更多
基金supported by the National Key R&D Program of China(2020YFA0406104,2020YFA0406101)the National MCF Energy R&D Program of China(2018YFE0306105)+5 种基金the Innovative Research Group Project of the National Natural Science Foundation of China(51821002)the National Natural Science Foundation of China(51725204,21771132,51972216,52041202)the Natural Science Foundation of Jiangsu Province(BK20190041)the Key-Area Research and Development Program of Guang Dong Province(2019B010933001)the Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Project。
文摘The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.
基金Supported by the National Natural Science Foundation of China under Grant No 51171027
文摘The growth kinetics of spherical NiAl and CuZr crystals are studied by using molecular dynamics simulations. The growth rates of crystals are found to increase with the grain radius. The simulations show that the interface thickness and the Jackson α-faetor increase as the growth proceeds, indicating that the interface becomes increasingly rough during growth. Due to the increasing interface roughening, the fraction of repeatable growth sites at interface f is proposed to actually increase in growth. An attachment rate, which is defined as the fraction of atoms that join the crystal interface without leaving, is used to approximate f, displaying a linear increase. With this approximation, we predict the growth rates as a function of the crystal radius, and the results qualitatively agree with those from the direct simulations.
基金supported by the National Natural Science Foundation of China(52202261)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ 14)Taishan Scholar Young Talent Program(tsqn201909114).
文摘Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.
基金This work was financially supported by Natural Science Foundation of Jiangsu Province(BK20210480)Hong Kong Scholars Program(P0035017).
文摘Carbon cloth(CC)-based electrodes have attracted extensive attention for next-generation wearable energy-storage devices due to their excellent electrical conductivity and mechanical flexibility.However,the application of conventional CC-based electrodes for zinc(Zn)storage severely hinders Zn ion transport and induces deleterious Zn dendrite growth,resulting in poor electrochemical reliability.Herein,a novel oxygen plasma-treated carbon cloth(OPCC)is rationally designed as a current collector for flexible hybrid Zn ion supercapacitors(ZISs).The modified interface of OPCC with abundant oxygenated groups enables enhanced electrolyte wettability and uniform superficial electric field distribution.A prolonged working lifespan for Zn electrodeposition is achieved by the OPCC due to the improved interfacial kinetics and homogenized ion gradient.The as-prepared hybrid ZIS also delivers excellent cycling endurance(98.5%capacity retention for 1500 cycles)with outstanding operation stability under various extreme conditions.This facile surface modification strategy provides a new way for developing future flexible electrodes for wearable electronic products.
基金the National Natural Science Foundation of China(Nos.51802171 and 52072197)Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)+1 种基金Taishan Scholar Young Talent Program(No.tsqn201909114)Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09).
文摘To conquer severe dendrites formation and side reactions of zinc metal anodes,which are serious obstacles for the practical applications of aqueous zinc ion battery(ZIB),herein,we develop a sodium allysulfonate(SAS)and acrylamide(AM)copolymer by radical polymerization process(crosslinking of C=C)as solid-state electrolyte.The interface kinetics is improved remarkably due to the high adhesion and excellent ion transferability of AM-SAS(AS)copolymers.Especially the sulfonic acid group in the hydrogel electrolyte can enhance the internal ionic conductivity effectively benefiting from its high affinity to Zn^(2+).Also,polymer chains realize re-regulation to Zn^(2+)flow in atomic-scale,thus leading to controllable deposition of Zn onto the dendrite-free Zn anodes.Consequently,the AS-1.5 electrolyte achieves ultra-stable Zn deposition/stripping behaviors with the lifespan over 1,000 h via the suppression of side-reactions and paralleled Zn deposition.High performances of Zn/Mn-doped V_(2)O_(5)(MnVO)(over 500 cycles)and Zn/diquinoxalino[2,3-a:2',3'-c]phenazine(HATN)(over 2,500 cycles)full cells demonstrate that the AS hydrogel electrolyte is a common approach for ZIBs under various conditions.This molecular regulation engineering opens a novel route for hydrogel electrolyte fabrication,where sulfonic groups perform as media of Zn^(2+)transfer.Therefore,high bulk ionic conductivity as well as excellent interface ion diffusion ability is obtained.
