Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving th...Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving the three-dimensional(3 D)highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al)crystals onto multi-walled carbon nanotubes(MWCNTs).Such 3 D hierarchically nanoporous web(3 D MIL-68(Al)@MWCNTs web)with a very high surface area,a large amount of micropores,electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron transportation.Molecular dynamic calculation confirmed the strong affinity of MIL-68(Al)for the adsorption of polyselenides,quite suitable for Li-Se battery.Their hexahedral channels(1.56 nm)are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels(0.63 nm).All these excellent characteristics of 3 D MIL-68(Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al)host by MWCNTs result in a high capacity of 453 m Ah/g at 0.2 C with 99.5%coulombic efficiency after 200 cycles with significantly improved cycle stability and rate performance.The 3 D MIL-68(Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework(MOF)based or MOF derived porous carbons used in Li-Se battery.展开更多
The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boos...The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boost textural,optical and electronic properties and photocurrent of TiO_(2) for high performance visible light H2 production from water splitting has been comprehensively investigated.Carbon doping can significantly increase the thermal stability,thus inhibiting the phase transformation of the Titania material from anatase to rutile while carbon coating can suppress the grain aggregation of TiO_(2).The synergy of carbon doping and coating can not only ensure an enhanced narrowing effect of the electronic band gap of TiO_(2) thus extending the absorption of photocatalysts to the visible regions,but also promote dramatically the separation of electron-hole pairs.Owing to these synergistic effects,the carbon coated and doped TiO_(2) shows much superior photocatalytic activity for both degradation of organics and photocatalytic/photoelectro chemical(PEC)water splitting under simulated sunlight illumination.The photocatalytic activity of obtained materials can reach 5,4 and 2 times higher than that of pristine TiO_(2),carbon doped TiO_(2) and carbon coated TiO_(2),respectively in the degradation of organic pollutants.The carbon coated and doped TiO_(2) materials exhibited more than 37 times and hundreds of times photocurrent enhancement under simulated sunlight and visible light,respectively compared to that of pristine TiO_(2).The present work providing new comprehensive understanding on carbon coating and doping effect could be very helpful for the development of advanced TiO_(2) materials for a large series of applications.展开更多
基金supported by the National Postdoctoral Program(2020M672782)National Natural Science Foundation of China(No.U1663225)+2 种基金Changjiang Scholars and Innovative Research Team in University(No.IRT15R52)National 111 project from the Ministry of Science and Technologythe Ministry of Education of China and the National Key R&D Program of China(No.2016YFA0202602)。
文摘Lithium-selenium(Li-Se)battery has attracted growing attention.Nevertheless,its practical application is still impeded by the shuttle effect of the formed polyselenides.Herein,we report in-situ hydrothermal weaving the three-dimensional(3 D)highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al)crystals onto multi-walled carbon nanotubes(MWCNTs).Such 3 D hierarchically nanoporous web(3 D MIL-68(Al)@MWCNTs web)with a very high surface area,a large amount of micropores,electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron transportation.Molecular dynamic calculation confirmed the strong affinity of MIL-68(Al)for the adsorption of polyselenides,quite suitable for Li-Se battery.Their hexahedral channels(1.56 nm)are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels(0.63 nm).All these excellent characteristics of 3 D MIL-68(Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al)host by MWCNTs result in a high capacity of 453 m Ah/g at 0.2 C with 99.5%coulombic efficiency after 200 cycles with significantly improved cycle stability and rate performance.The 3 D MIL-68(Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework(MOF)based or MOF derived porous carbons used in Li-Se battery.
基金supported by the National Natural Science Foundation of China(U1663225,21805280)Program for Changjiang Scholars and Innovative Research Team in University(IRT15R52)+2 种基金the Minstry of Education of Chinathe 111 Project(Grant No.B20002)from the Ministry of Science and Technology and the Ministry of Education of China,China,European Commission,Interreg V France-Wallonie-Vlaanderen(Depollutair)the Fundamental Research Funds for the Central Universities(WUT:2017III001),Chinathe FJIRSM&IUE Joint Research Fund(RHZX-2018-002),China for supporting this work。
文摘The"one pot"simultaneous carbon coating and doping of TiO_(2) materials by the hydrolysis of TiCl4 in fructose is reported.The synergistic effect of carbon doping and coating of TiO_(2) to significantly boost textural,optical and electronic properties and photocurrent of TiO_(2) for high performance visible light H2 production from water splitting has been comprehensively investigated.Carbon doping can significantly increase the thermal stability,thus inhibiting the phase transformation of the Titania material from anatase to rutile while carbon coating can suppress the grain aggregation of TiO_(2).The synergy of carbon doping and coating can not only ensure an enhanced narrowing effect of the electronic band gap of TiO_(2) thus extending the absorption of photocatalysts to the visible regions,but also promote dramatically the separation of electron-hole pairs.Owing to these synergistic effects,the carbon coated and doped TiO_(2) shows much superior photocatalytic activity for both degradation of organics and photocatalytic/photoelectro chemical(PEC)water splitting under simulated sunlight illumination.The photocatalytic activity of obtained materials can reach 5,4 and 2 times higher than that of pristine TiO_(2),carbon doped TiO_(2) and carbon coated TiO_(2),respectively in the degradation of organic pollutants.The carbon coated and doped TiO_(2) materials exhibited more than 37 times and hundreds of times photocurrent enhancement under simulated sunlight and visible light,respectively compared to that of pristine TiO_(2).The present work providing new comprehensive understanding on carbon coating and doping effect could be very helpful for the development of advanced TiO_(2) materials for a large series of applications.