It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized pheno...It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized phenolic resin spheres via suspension polymerization were carbonized and activated by water vapor to obtain activated carbon spheres(ACSs).Subsequently,Bi_(2)MoO_(6)/ACSs were prepared via hydrothermal-impregnated method.The systematical characterizations of samples,including XRD,XPS,SEM,EDX,DRS,BET,PL,CO_(2) adsorption isotherm,EIS and transient photocurrent,were analyzed.The results clearly demonstrated that Bi_(2)MoO_(6) with suitable oxidation reduction potentials and bandgap and ACSs with admirable CO_(2) adsorption and electrical conductivity not only enhanced separation efficiency of photoindued electron-hole pair,but also displayed as 1.8 times CO_(2) reduction activity to CO as single Bi_(2)MoO_(6) sample under Xe-lamp irradiation.Finally,a concerned photocatalytic CO_(2) reduction mechanism was proposed and investigated.Our findings should provide innovative guidance for designing a series of photocatalytic CO_(2) reduction materials with highly efficient and selective ability.展开更多
As an effective means to improve charge carrier separation efficiency and directional transport,the gradient doping of foreign elements to build multi-homojunction structures inside catalysts has received wide attenti...As an effective means to improve charge carrier separation efficiency and directional transport,the gradient doping of foreign elements to build multi-homojunction structures inside catalysts has received wide attentions.Herein,we reported a simple and robust method to construct multi-homojunctions in black TiO_(2) nanotubes by the gradient doping of Ni species through the diffusion of deposited Ni element on the top of black TiO2 nanotubes driven by a high temperature annealing process.The gradient Ni distribution created parts of different Fermi energy levels and energy band structures within the same black TiO_(2) nanotube,which subsequently formed two series of multi-homojunctions within it.This special multi-homojunction structure largely enhanced the charge carrier separation and transportation,while the low concentration of defect states near the surface layer further inhibited carrier recombination and facilitated the surface reaction.Thus,the B-TNT-2Ni sample with the optimized Ni doping concentration exhibited an enhanced hydrogen evolution rate of~1.84 mmol·g^(−1)·h^(−1)under visible light irradiation without the assistance of noble-metal cocatalysts,~four times higher than that of the pristine black TiO_(2)nanotube array.With the capability to create multi-homojunction structures,this approach could be readily applied to various dopant systems and catalyst materials for a broad range of technical applications.展开更多
Photocatalytic non-oxidative coupling of methane(PNOCM)is a mild and cost-effective method for the production of multicarbon compounds.However,the separation of photogenerated charges and activation of methane(CH4)are...Photocatalytic non-oxidative coupling of methane(PNOCM)is a mild and cost-effective method for the production of multicarbon compounds.However,the separation of photogenerated charges and activation of methane(CH4)are the main challenges for this reaction.Here,single crystal-like TiO_(2) nanotubes(VO-p-TNTs)with oxygen vacancies(VO)and preferential orientation were prepared and applied to PNOCM.The results demonstrate that the significantly enhanced photocatalytic performance is mainly related to the strong synergistic effect between preferential orientation and VO.The preferential orientation of VO-p-TNT along the[001]direction reduces the formation of complex centers at grain boundaries as the form of interfacial states and potential barriers,which improves the separation and transport of photogenerated carriers.Meanwhile,VO provides abundant coordination unsaturated sites for CH4 chemisorption and also acts as electron traps to hinder the recombination of electrons and holes,establishing an effective electron transfer channel between the adsorbed CH4 molecule and photocatalyst,thus weakening the C–H bond.In addition,the introduction of VO broadens the light absorption range.As a result,VO-p-TNT exhibits excellent PNOCM performance and provides new insights into catalyst design for CH4 conversion.展开更多
Effective charge separation and transfer is deemed to be the contributing factor to achieve high photoelectrochemical(PEC)water splitting performance on photoelectrodes.Building a phase junction structure with control...Effective charge separation and transfer is deemed to be the contributing factor to achieve high photoelectrochemical(PEC)water splitting performance on photoelectrodes.Building a phase junction structure with controllable phase transition of WO_(3) can further improve the photocatalytic performance.In this work,we realized the transition from orthorhombic to monoclinic by regulating the annealing temperatures,and constructed an orthorhombic–monoclinic WO_(3)(o-WO_(3)/m-WO_(3))phase junction.The formation of oxygen vacancies causes an imbalance of the charge distribution in the crystal structure,which changes the W–O bond length and bond angle,accelerating the phase transition.As expected,an optimum PEC activity was achieved over the o-WO_(3)/m-WO_(3) phase junction in WO_(3)-450 photoelectrode,yielding the maximum O_(2) evolution rate roughly 32 times higher than that of pure WO_(3)-250 without any sacrificial agents under visible light irradiation.The enhancement of catalytic activity is attributed to the atomically smooth interface with a highly matched lattice and robust built-in electric field around the phase junction,which leads to a less-defective and abrupt interface and provides a smooth interfacial charge separation and transfer path,leading to improved charge separation and transfer efficiency and a great enhancement in photocatalytic activity.This work strikes out on new paths in the formation of an oxygen vacancy-induced phase transition and provides new ideas for the design of catalysts.展开更多
Electrocatalytic reduction of Cr(Ⅵ)to less toxic Cr(Ⅲ)is deemed as a promising technique.Conventional electrocatalytic reduction is always driven by a constant cathodic potential,which exhibits a repelling action to...Electrocatalytic reduction of Cr(Ⅵ)to less toxic Cr(Ⅲ)is deemed as a promising technique.Conventional electrocatalytic reduction is always driven by a constant cathodic potential,which exhibits a repelling action to Cr(Ⅵ)oxyanions in wastewater and consequently suppresses reduction kinetics.In order to remarkably accelerate Cr(Ⅵ)electrocatalytic reduction,we applied a pulsed potential on an Fe^(2+)-NiFe LDH/NF electrode synthesized by in situ growth of Fe^(2+)-doped NiFe LDH nanosheets on Ni foam using a spontaneous redox reaction.Under anodic potential section,HCrO_(4)^(–) anions are adsorbed on the electrode surface and reduced to Cr(Ⅲ)by Fe^(2+).Then,Cr(Ⅲ)ions are desorbed from the electrode surface under coulombic force.The regeneration of Fe^(2+) and direct reduction of Cr(Ⅵ)are achieved under cathodic potential section.The pulsed potential can achieve complete elimination of Cr(Ⅵ)within 60 min at an initial concentration of 10 mg L^(-1),and the removal efficiency shows a 60%increase with respect to that under constant cathodic potential.展开更多
Epidemics of emerging and neglected infectious diseases are severe threats to public health and are largely driven by the promotion of globalization and by international multi-border cooperation.Mosquitoborne viruses ...Epidemics of emerging and neglected infectious diseases are severe threats to public health and are largely driven by the promotion of globalization and by international multi-border cooperation.Mosquitoborne viruses are among the most important agents of these diseases,with an associated mortality of over one million people worldwide(1).The well-known mosquito-borne diseases(MBDs)with global scale include malaria,dengue fever,chikungunya.展开更多
基金The authors are thankful to the National Natural Science Foundation of China(No.21978196,21676178,21706179)Shanxi Province Science Foundation for Youths(201801D211008).
文摘It is rather essential to design glorious system with high CO_(2) adsorption capacity and electron migration efficiency for improving selective and effective CO_(2) reduction into solar fuels.Here,as-synthesized phenolic resin spheres via suspension polymerization were carbonized and activated by water vapor to obtain activated carbon spheres(ACSs).Subsequently,Bi_(2)MoO_(6)/ACSs were prepared via hydrothermal-impregnated method.The systematical characterizations of samples,including XRD,XPS,SEM,EDX,DRS,BET,PL,CO_(2) adsorption isotherm,EIS and transient photocurrent,were analyzed.The results clearly demonstrated that Bi_(2)MoO_(6) with suitable oxidation reduction potentials and bandgap and ACSs with admirable CO_(2) adsorption and electrical conductivity not only enhanced separation efficiency of photoindued electron-hole pair,but also displayed as 1.8 times CO_(2) reduction activity to CO as single Bi_(2)MoO_(6) sample under Xe-lamp irradiation.Finally,a concerned photocatalytic CO_(2) reduction mechanism was proposed and investigated.Our findings should provide innovative guidance for designing a series of photocatalytic CO_(2) reduction materials with highly efficient and selective ability.
基金support is gratefully acknowledged from the National Natural Science Foundation of China(NSFC)(Nos.62004137,21878257,and 21978196)the Natural Science Foundation(NSF)of Shanxi Province(No.20210302123102)+4 种基金the Key Research and Development Program of Shanxi Province(No.201803D421079)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(No.2019L0156)the Research Project Supported by Shanxi Scholarship Council of China(No.2020-050)the Fundamental Research Funds for the Central Universities(No.2682021CX116)Sichuan Science and Technology Program(No.2020YJ0259).
文摘As an effective means to improve charge carrier separation efficiency and directional transport,the gradient doping of foreign elements to build multi-homojunction structures inside catalysts has received wide attentions.Herein,we reported a simple and robust method to construct multi-homojunctions in black TiO_(2) nanotubes by the gradient doping of Ni species through the diffusion of deposited Ni element on the top of black TiO2 nanotubes driven by a high temperature annealing process.The gradient Ni distribution created parts of different Fermi energy levels and energy band structures within the same black TiO_(2) nanotube,which subsequently formed two series of multi-homojunctions within it.This special multi-homojunction structure largely enhanced the charge carrier separation and transportation,while the low concentration of defect states near the surface layer further inhibited carrier recombination and facilitated the surface reaction.Thus,the B-TNT-2Ni sample with the optimized Ni doping concentration exhibited an enhanced hydrogen evolution rate of~1.84 mmol·g^(−1)·h^(−1)under visible light irradiation without the assistance of noble-metal cocatalysts,~four times higher than that of the pristine black TiO_(2)nanotube array.With the capability to create multi-homojunction structures,this approach could be readily applied to various dopant systems and catalyst materials for a broad range of technical applications.
基金The financial support was gratefully acknowledged from the National Natural Science Foundation of China(Grant Nos.62004137,21878257,and 21978196)Natural Science Foundation of Shanxi Province(Grant No.20210302123102)+3 种基金Key Research and Development Program of Shanxi Province(Grant No.201803D421079)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(Grant No.2019L0156)Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(Grant No.2022SX-TD002)Research Project Supported by Shanxi Scholarship Council of China(Grant No.2020-050).
文摘Photocatalytic non-oxidative coupling of methane(PNOCM)is a mild and cost-effective method for the production of multicarbon compounds.However,the separation of photogenerated charges and activation of methane(CH4)are the main challenges for this reaction.Here,single crystal-like TiO_(2) nanotubes(VO-p-TNTs)with oxygen vacancies(VO)and preferential orientation were prepared and applied to PNOCM.The results demonstrate that the significantly enhanced photocatalytic performance is mainly related to the strong synergistic effect between preferential orientation and VO.The preferential orientation of VO-p-TNT along the[001]direction reduces the formation of complex centers at grain boundaries as the form of interfacial states and potential barriers,which improves the separation and transport of photogenerated carriers.Meanwhile,VO provides abundant coordination unsaturated sites for CH4 chemisorption and also acts as electron traps to hinder the recombination of electrons and holes,establishing an effective electron transfer channel between the adsorbed CH4 molecule and photocatalyst,thus weakening the C–H bond.In addition,the introduction of VO broadens the light absorption range.As a result,VO-p-TNT exhibits excellent PNOCM performance and provides new insights into catalyst design for CH4 conversion.
基金The financial support is gratefully acknowledged from the National Natural Science Foundation of China(Grant Nos.62004137,21878257,and 21978196)Natural Science Foundation of Shanxi Province(Grant No.20210302123102)+4 种基金Key Research and Development Program of Shanxi Province(Grant No.201803D421079)Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(Grant No.2019L0156)Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(Grant No.2022SX-TD002)Shanxi Provincial Key Innovative Research Team in Science and Technology(Grant No.201605D13104510)Research Project Supported by Shanxi Scholarship Council of China(Grant No.2020-050).
文摘Effective charge separation and transfer is deemed to be the contributing factor to achieve high photoelectrochemical(PEC)water splitting performance on photoelectrodes.Building a phase junction structure with controllable phase transition of WO_(3) can further improve the photocatalytic performance.In this work,we realized the transition from orthorhombic to monoclinic by regulating the annealing temperatures,and constructed an orthorhombic–monoclinic WO_(3)(o-WO_(3)/m-WO_(3))phase junction.The formation of oxygen vacancies causes an imbalance of the charge distribution in the crystal structure,which changes the W–O bond length and bond angle,accelerating the phase transition.As expected,an optimum PEC activity was achieved over the o-WO_(3)/m-WO_(3) phase junction in WO_(3)-450 photoelectrode,yielding the maximum O_(2) evolution rate roughly 32 times higher than that of pure WO_(3)-250 without any sacrificial agents under visible light irradiation.The enhancement of catalytic activity is attributed to the atomically smooth interface with a highly matched lattice and robust built-in electric field around the phase junction,which leads to a less-defective and abrupt interface and provides a smooth interfacial charge separation and transfer path,leading to improved charge separation and transfer efficiency and a great enhancement in photocatalytic activity.This work strikes out on new paths in the formation of an oxygen vacancy-induced phase transition and provides new ideas for the design of catalysts.
基金financially supported by the National Natural Science Foundation of China(NSFC)(Nos.62004137,21878257 and 21978196)the Natural Science Foundation(NSF)of Shanxi Province(No.201701D221083)+5 种基金the Key Research and Development Program of Shanxi Province(No.201803D421079)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(No.2019L0156)the Shanxi Provincial Key Innovative Research Team in Science and Technology(No.201605D131045–10)the Research Project Supported by Shanxi Scholarship Council of China(2020–050)Horizontal Project(203010675-J)Liaoning Baiqianwan Talents Program。
文摘Electrocatalytic reduction of Cr(Ⅵ)to less toxic Cr(Ⅲ)is deemed as a promising technique.Conventional electrocatalytic reduction is always driven by a constant cathodic potential,which exhibits a repelling action to Cr(Ⅵ)oxyanions in wastewater and consequently suppresses reduction kinetics.In order to remarkably accelerate Cr(Ⅵ)electrocatalytic reduction,we applied a pulsed potential on an Fe^(2+)-NiFe LDH/NF electrode synthesized by in situ growth of Fe^(2+)-doped NiFe LDH nanosheets on Ni foam using a spontaneous redox reaction.Under anodic potential section,HCrO_(4)^(–) anions are adsorbed on the electrode surface and reduced to Cr(Ⅲ)by Fe^(2+).Then,Cr(Ⅲ)ions are desorbed from the electrode surface under coulombic force.The regeneration of Fe^(2+) and direct reduction of Cr(Ⅵ)are achieved under cathodic potential section.The pulsed potential can achieve complete elimination of Cr(Ⅵ)within 60 min at an initial concentration of 10 mg L^(-1),and the removal efficiency shows a 60%increase with respect to that under constant cathodic potential.
基金The Special Foundation of Basic Science and Technology Resources Survey of Ministry of Science and Technology of China(No.2017FY101200)The Open Project of Key Laboratory of Parasite and Vector Biology,China Ministry of Health(No.WSBKFKT-201804)and The Fifth Round of Three-Year Public Health Action Plan of Shanghai(No.GWV-10.1-XK13).
文摘Epidemics of emerging and neglected infectious diseases are severe threats to public health and are largely driven by the promotion of globalization and by international multi-border cooperation.Mosquitoborne viruses are among the most important agents of these diseases,with an associated mortality of over one million people worldwide(1).The well-known mosquito-borne diseases(MBDs)with global scale include malaria,dengue fever,chikungunya.