Photoactive WO3is attractive as a photocatalyst for green energy evolution through water splitting.In the present work,an electrochemical anodic oxidation method was used to fabricate a photo‐responsive nanotube arra...Photoactive WO3is attractive as a photocatalyst for green energy evolution through water splitting.In the present work,an electrochemical anodic oxidation method was used to fabricate a photo‐responsive nanotube array‐like WO3/W(NA‐WO3/W)photoanode from W foil as a precursor.Compared with a reference commercial WO3/W electrode,the NA‐WO3/W photoanode exhibited enhanced and stable photoelectrocatalytic(PEC)activity for visible‐light‐driven water splitting with a typical H2/O2stoichiometric ratio of2:1and quantum efficiency of approximately5.23%under visible‐light irradiation from a light‐emitting diode(λ=420nm,15mW/cm2).The greatly enhanced PEC performance of the NA‐WO3/Wphotoanode was attributed to its fast electron–hole separation rate,which resulted from the one‐dimensional nanotube array‐like structure,high crystallinity of monoclinic WO3,and strong interaction between WO3and W foil.This work paves the way to a facile route to prepare highly active photoelectrodes for solar light transfer to chemical energy.展开更多
Exploration of cost-effective electrocatalysts for boosting the overall water-splitting efficiency is vitally important for obtaining renewable fuels such as hydrogen.Here,earth-abundant CoxNi1-xO nanowire arrays were...Exploration of cost-effective electrocatalysts for boosting the overall water-splitting efficiency is vitally important for obtaining renewable fuels such as hydrogen.Here,earth-abundant CoxNi1-xO nanowire arrays were used as a structural framework to dilute Ir incorporation for fabricating electrocatalysts for water splitting.Minimal Ir-incorporated CoxNi1-xO nanowire arrays were synthesized through the facile hydrothermal method with subsequent calcination by using Ni foam(NF)as both the substrate and source of Ni.The electrocatalytic water-splitting performance was found to crucially depend on the Ir content of the parent CoxNi1-xO nanowire arrays.As a result,for a minimal Ir content,as low as 0.57 wt%,the obtained Ir-CoxNi1-xO/NF electrodes exhibited optimal catalytic activity in terms of a low overpotential of 260 mV for the oxygen evolution reaction and 53 mV for the hydrogen evolution reaction at 10 mA cm?2 in 1 mol L–1 KOH.When used as bifunctional electrodes in water splitting,the current density of 10 mA cm–2 was obtained at a low cell voltage of 1.55 V.Density functional theory calculations revealed that the Ir-doped CoxNi1-xO arrays exhibited enhanced electrical conductivity and low Gibbs free energy,which contributed to the improved electrocatalytic activity.The present study presents a new strategy for the development of transition metal oxide electrocatalysts with low levels of Ir incorporation for efficient water splitting.展开更多
Well‐aligned zinc oxide(ZnO)nanotube arrays loaded with tungsten trioxide(WO3)nanoparticles were synthesized by a process involving chemical bath deposition in combination with pyrolysis.The prepared ZnO–WO3composit...Well‐aligned zinc oxide(ZnO)nanotube arrays loaded with tungsten trioxide(WO3)nanoparticles were synthesized by a process involving chemical bath deposition in combination with pyrolysis.The prepared ZnO–WO3composites were characterized by X‐ray diffraction,energy dispersive spectrometer,field emission scanning electron microscopy,X‐ray photoelectron spectroscopy,photoluminescence spectroscopy,Fourier transform infrared spectroscopy and UV–vis diffuse reflectance spectroscopy.The photocatalytic activities of the ZnO–WO3composite photocatalysts with different WO3contents for the degradation of the herbicide chlorinated phenoxyacetic acid(MCPA‐Na)under simulated sunlight irradiation were systematically evaluated.It was found that the WO3content had a great effect on the photocatalytic activity of the ZnO–WO3composites.The composite with3%WO3showed the highest photocatalytic activity,with a degradation rate of chlorinated phenoxyacetic acid of98.5%after200min with20mg of photocatalyst.This photodegradation rate was about twice that of the pristine ZnO nanotube array.The recombination of photogenerated electrons and holes was increasingly suppressed with the addition of WO3to ZnO.The high relative content of defects on the surface of the ZnO–WO3composites was beneficial to their photocatalytic activity in the degradation of chlorinated phenoxyacetic acid.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
Well-ordered TiO 2 nanotube arrays (TNAs) were fabricated by electrochemical anodization in a mixed organic electrolyte consisting of ethylene glycol and glycerol. The morphology, structure, crystalline phase, and pho...Well-ordered TiO 2 nanotube arrays (TNAs) were fabricated by electrochemical anodization in a mixed organic electrolyte consisting of ethylene glycol and glycerol. The morphology, structure, crystalline phase, and photocatalytic properties of TNAs were characterized by using TEM, SEM, XRD and photodegradation of methylene blue. It was found that the morphology and structure of TNAs could be significantly influenced by the anodization time and applied voltage. The obtained tube length was found to be proportional to anodization time, and the calculated growth rate of nanotubes was 0.6 m/h. The microstructure analysis demonstrated that the diameter and thickness of the nanotubes increased with the increase of anodization voltage. The growth mechanism of TNAs was also proposed according to the observed relationship between current density and time during anodization. As expected, the obtained TNAs showed a higher photocatalytic activity than the commercial TiO 2 P25 nanoparticles.展开更多
The development of effective and low-cost catalysts for overall water splitting is essential for clean production of hydrogen from water.In this paper,we report the synthesis of cobalt-vanadium(Co-V)bimetal-based ca...The development of effective and low-cost catalysts for overall water splitting is essential for clean production of hydrogen from water.In this paper,we report the synthesis of cobalt-vanadium(Co-V)bimetal-based catalysts for the effective water splitting.The Co_2V_2O_7·xH_2O nanoplates containing both Co and V elements were selected as the precursors.After the calcination under NH_3atmosphere,the Co_2VO_4and Co/VN could be obtained just by tuning the calcination temperature.Electrochemical tests indicated that the Co-V bimetal-based materials could be used as active hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalyst by regulating their structure.The Co/VN showed good performance for HER with the onset potential of68 mV and can achieve a current density of 10 mA cm^(-2)at an overpotential of 92 m V.Meanwhile,the Co_2VO_4exhibited the obvious OER performance with overpotential of 300 mV to achieve a current density of 10 mA cm^(-2).When the Co_2VO_4and Co/VN were used as the anode and cathode in a twoelectrode system,respectively,the cell needed a voltage of1.65 V to achieve 10 mA cm^(-2)together with good stability.This work would be indicative to constructing Co-V bimetalbased catalysts for the catalytic application.展开更多
基金supported by the National Natural Science Foundation of China(21207090,21477079,21261140333)PCSIRT(IRT1269)a scheme administrated by Shanghai Normal University(DXL122,and S30406)~~
文摘Photoactive WO3is attractive as a photocatalyst for green energy evolution through water splitting.In the present work,an electrochemical anodic oxidation method was used to fabricate a photo‐responsive nanotube array‐like WO3/W(NA‐WO3/W)photoanode from W foil as a precursor.Compared with a reference commercial WO3/W electrode,the NA‐WO3/W photoanode exhibited enhanced and stable photoelectrocatalytic(PEC)activity for visible‐light‐driven water splitting with a typical H2/O2stoichiometric ratio of2:1and quantum efficiency of approximately5.23%under visible‐light irradiation from a light‐emitting diode(λ=420nm,15mW/cm2).The greatly enhanced PEC performance of the NA‐WO3/Wphotoanode was attributed to its fast electron–hole separation rate,which resulted from the one‐dimensional nanotube array‐like structure,high crystallinity of monoclinic WO3,and strong interaction between WO3and W foil.This work paves the way to a facile route to prepare highly active photoelectrodes for solar light transfer to chemical energy.
基金financially supported by the National Natural Science Foundation of China (51772255)the Hunan Provincial Innovation Foundation For Postgraduate (CX2017B274)+1 种基金the National Basic Research Program of China (2015CB921103)the Program for Changjiang Scholars and Innovative Research Team in University (IRT13093)~~
文摘Exploration of cost-effective electrocatalysts for boosting the overall water-splitting efficiency is vitally important for obtaining renewable fuels such as hydrogen.Here,earth-abundant CoxNi1-xO nanowire arrays were used as a structural framework to dilute Ir incorporation for fabricating electrocatalysts for water splitting.Minimal Ir-incorporated CoxNi1-xO nanowire arrays were synthesized through the facile hydrothermal method with subsequent calcination by using Ni foam(NF)as both the substrate and source of Ni.The electrocatalytic water-splitting performance was found to crucially depend on the Ir content of the parent CoxNi1-xO nanowire arrays.As a result,for a minimal Ir content,as low as 0.57 wt%,the obtained Ir-CoxNi1-xO/NF electrodes exhibited optimal catalytic activity in terms of a low overpotential of 260 mV for the oxygen evolution reaction and 53 mV for the hydrogen evolution reaction at 10 mA cm?2 in 1 mol L–1 KOH.When used as bifunctional electrodes in water splitting,the current density of 10 mA cm–2 was obtained at a low cell voltage of 1.55 V.Density functional theory calculations revealed that the Ir-doped CoxNi1-xO arrays exhibited enhanced electrical conductivity and low Gibbs free energy,which contributed to the improved electrocatalytic activity.The present study presents a new strategy for the development of transition metal oxide electrocatalysts with low levels of Ir incorporation for efficient water splitting.
基金supported by the National Natural Science Foundation of China(51574071)~~
文摘Well‐aligned zinc oxide(ZnO)nanotube arrays loaded with tungsten trioxide(WO3)nanoparticles were synthesized by a process involving chemical bath deposition in combination with pyrolysis.The prepared ZnO–WO3composites were characterized by X‐ray diffraction,energy dispersive spectrometer,field emission scanning electron microscopy,X‐ray photoelectron spectroscopy,photoluminescence spectroscopy,Fourier transform infrared spectroscopy and UV–vis diffuse reflectance spectroscopy.The photocatalytic activities of the ZnO–WO3composite photocatalysts with different WO3contents for the degradation of the herbicide chlorinated phenoxyacetic acid(MCPA‐Na)under simulated sunlight irradiation were systematically evaluated.It was found that the WO3content had a great effect on the photocatalytic activity of the ZnO–WO3composites.The composite with3%WO3showed the highest photocatalytic activity,with a degradation rate of chlorinated phenoxyacetic acid of98.5%after200min with20mg of photocatalyst.This photodegradation rate was about twice that of the pristine ZnO nanotube array.The recombination of photogenerated electrons and holes was increasingly suppressed with the addition of WO3to ZnO.The high relative content of defects on the surface of the ZnO–WO3composites was beneficial to their photocatalytic activity in the degradation of chlorinated phenoxyacetic acid.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金financially supported by the National Natural Science Foundation of China (51072189, 21003111, 21003112)Natural Science Foundation of Zhejiang Province (Y4090507)Scientific Research Foundation of Education Department of Zhejiang Province(Y201018867)
文摘Well-ordered TiO 2 nanotube arrays (TNAs) were fabricated by electrochemical anodization in a mixed organic electrolyte consisting of ethylene glycol and glycerol. The morphology, structure, crystalline phase, and photocatalytic properties of TNAs were characterized by using TEM, SEM, XRD and photodegradation of methylene blue. It was found that the morphology and structure of TNAs could be significantly influenced by the anodization time and applied voltage. The obtained tube length was found to be proportional to anodization time, and the calculated growth rate of nanotubes was 0.6 m/h. The microstructure analysis demonstrated that the diameter and thickness of the nanotubes increased with the increase of anodization voltage. The growth mechanism of TNAs was also proposed according to the observed relationship between current density and time during anodization. As expected, the obtained TNAs showed a higher photocatalytic activity than the commercial TiO 2 P25 nanoparticles.
基金supported by the Key Program Projects of the National Natural Science Foundation of China (21631004)the National Natural Science Foundation of China (21601055, 21571054 and 21401048)+1 种基金the Natural Science Foundation of Heilongjiang Province (B2017008)Heilongjiang University Excellent Youth Foundation
文摘The development of effective and low-cost catalysts for overall water splitting is essential for clean production of hydrogen from water.In this paper,we report the synthesis of cobalt-vanadium(Co-V)bimetal-based catalysts for the effective water splitting.The Co_2V_2O_7·xH_2O nanoplates containing both Co and V elements were selected as the precursors.After the calcination under NH_3atmosphere,the Co_2VO_4and Co/VN could be obtained just by tuning the calcination temperature.Electrochemical tests indicated that the Co-V bimetal-based materials could be used as active hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalyst by regulating their structure.The Co/VN showed good performance for HER with the onset potential of68 mV and can achieve a current density of 10 mA cm^(-2)at an overpotential of 92 m V.Meanwhile,the Co_2VO_4exhibited the obvious OER performance with overpotential of 300 mV to achieve a current density of 10 mA cm^(-2).When the Co_2VO_4and Co/VN were used as the anode and cathode in a twoelectrode system,respectively,the cell needed a voltage of1.65 V to achieve 10 mA cm^(-2)together with good stability.This work would be indicative to constructing Co-V bimetalbased catalysts for the catalytic application.