Photoelectrochemical NO_(3)^(-)reduction(PEC NITRR)not only provides a promising solution for promoting the global nitrogen cycle,but also converts NO_(3)^(-)to the important chemicals(NH_(3)).However,it is still a gr...Photoelectrochemical NO_(3)^(-)reduction(PEC NITRR)not only provides a promising solution for promoting the global nitrogen cycle,but also converts NO_(3)^(-)to the important chemicals(NH_(3)).However,it is still a great challenge to prepare catalysts with excellent NO_(3)^(-)adsorption/activation capacity to achieve high NITRR.Herein,we designed a novel Fe^(2+)~Cu^(2+)Fe^(3+)LDH/BiVO_(4)(FCF-LDH/BVO)catalyst with synergistic effect of chemical adsorption and physical enrichment.Fe^(2+)in FCF-LDH/BVO provides the rich Lewis acid sites for the adsorption of NO_(3)^(-),and the appropriate layer spacing of FCF-LDH further promotes the physical enrichment of NO_(3)^(-)in its interior,thus realizing the effective contact between NO_(3)^(-)and active sites(Fe^(2+)).FCF-LDH/BVO showed excellent NH_(3)production performance(FE_(NH_(3))=66.1%,r_(NH_(3))=13.8μg h^(-1)cm^(-2))and selectivity(FE_(NO_(2)^(-))=2.5%,r_(NO_(2)^(-))=4.9μg h^(-1)cm^(-2))in 0.5 mol L^(-1)Na_(2)SO_(4)electrolyte.In addition,FCF-LDH/BVO maintains the desirable PEC stability for six cycle experiments,showing great potential for practical application.The^(14)NO_(3)^(-)and^(15)NO_(3)^(-)isotope test provides strong evidence for further verification of the origin of N in the generated NH_(3).This LDH catalyst has a great potential in PEC removal of NO_(3)^(-)from groundwater.展开更多
Here we report the WO3 thin films on F-doped SnO2 conducting glass (FTO) substrates which were prepared by using dip film-drawing method. Dip film-drawing was a simple, convenient, economical method and in largescale ...Here we report the WO3 thin films on F-doped SnO2 conducting glass (FTO) substrates which were prepared by using dip film-drawing method. Dip film-drawing was a simple, convenient, economical method and in largescale to prepare photoanodes for future applications. The FTO substrates were dipped in tungstic acid solution then film-drawn included 3, 6, 9, 12 and 15 times for prepared different thicknesses of WO3 thin film photoanodes. Then the photoa no des were employed as the electrodes in photoelectrochemical property Keywords: WO3 thin films Dip film-drawing Photoelectrochemical Thicknesses Large-scale measurements, which include scan linear sweep, repeated on/off illumination cycles, electrochemical impedanee spectroscopy and incident phot on to current conversion efficiency, respectively. The results showed that the WO3 thin films dipped 9 times with 175 nm thicknesses had the best photoelectrochemical performance of 0.067 mA·cm^-2 at 1.23 V versus RHE.展开更多
Decoration of metal-organic framework(MOF)has been considered as an effective route to improve the photoelectrochemical(PEC)performance of TiO_(2),but there is still a lack of understanding of the regulatory structure...Decoration of metal-organic framework(MOF)has been considered as an effective route to improve the photoelectrochemical(PEC)performance of TiO_(2),but there is still a lack of understanding of the regulatory structure.Herein,Ni-MOF was rationally introduced by in-situ etching method,which helps for artificially regulating the coordination state of Ni sites.The photocurrent density(0.81 mA/cm^(2))and IPCE value(33.1%)of TiO_(2)-MOF-2 are about twice higher than that of pristine TiO_(2) due to the rich unsaturated sites of Ni-MOF.Meanwhile,the saturated coordination has caused the decline of PEC performance because of the obvious steric hindrance.Therefore,this work presents an insight for the effect of coordination state on PEC activity especially in MOF system.展开更多
基金National Natural Science Foundation of China(22075112)Jiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural Equipment(XTCX2027)Jiangsu Province Innovation Support Program International Science and Technology Cooperation Project(BZ2022045)。
文摘Photoelectrochemical NO_(3)^(-)reduction(PEC NITRR)not only provides a promising solution for promoting the global nitrogen cycle,but also converts NO_(3)^(-)to the important chemicals(NH_(3)).However,it is still a great challenge to prepare catalysts with excellent NO_(3)^(-)adsorption/activation capacity to achieve high NITRR.Herein,we designed a novel Fe^(2+)~Cu^(2+)Fe^(3+)LDH/BiVO_(4)(FCF-LDH/BVO)catalyst with synergistic effect of chemical adsorption and physical enrichment.Fe^(2+)in FCF-LDH/BVO provides the rich Lewis acid sites for the adsorption of NO_(3)^(-),and the appropriate layer spacing of FCF-LDH further promotes the physical enrichment of NO_(3)^(-)in its interior,thus realizing the effective contact between NO_(3)^(-)and active sites(Fe^(2+)).FCF-LDH/BVO showed excellent NH_(3)production performance(FE_(NH_(3))=66.1%,r_(NH_(3))=13.8μg h^(-1)cm^(-2))and selectivity(FE_(NO_(2)^(-))=2.5%,r_(NO_(2)^(-))=4.9μg h^(-1)cm^(-2))in 0.5 mol L^(-1)Na_(2)SO_(4)electrolyte.In addition,FCF-LDH/BVO maintains the desirable PEC stability for six cycle experiments,showing great potential for practical application.The^(14)NO_(3)^(-)and^(15)NO_(3)^(-)isotope test provides strong evidence for further verification of the origin of N in the generated NH_(3).This LDH catalyst has a great potential in PEC removal of NO_(3)^(-)from groundwater.
基金Supported by the National Natural Science Foundation of China(21522603,21477050,21401082,21503142,21671083)Six Talent Peaks Project in Jiangsu Province(XCL-025)+2 种基金and the Chinese-German Cooperation Research Project(GZ1091)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX17_1774)the Excellent Youth Foundation of Jiangsu Scientific Committee(BK20170526)
文摘Here we report the WO3 thin films on F-doped SnO2 conducting glass (FTO) substrates which were prepared by using dip film-drawing method. Dip film-drawing was a simple, convenient, economical method and in largescale to prepare photoanodes for future applications. The FTO substrates were dipped in tungstic acid solution then film-drawn included 3, 6, 9, 12 and 15 times for prepared different thicknesses of WO3 thin film photoanodes. Then the photoa no des were employed as the electrodes in photoelectrochemical property Keywords: WO3 thin films Dip film-drawing Photoelectrochemical Thicknesses Large-scale measurements, which include scan linear sweep, repeated on/off illumination cycles, electrochemical impedanee spectroscopy and incident phot on to current conversion efficiency, respectively. The results showed that the WO3 thin films dipped 9 times with 175 nm thicknesses had the best photoelectrochemical performance of 0.067 mA·cm^-2 at 1.23 V versus RHE.
基金the Start Up Foundation of Jiangsu University(11JDG153).
文摘Decoration of metal-organic framework(MOF)has been considered as an effective route to improve the photoelectrochemical(PEC)performance of TiO_(2),but there is still a lack of understanding of the regulatory structure.Herein,Ni-MOF was rationally introduced by in-situ etching method,which helps for artificially regulating the coordination state of Ni sites.The photocurrent density(0.81 mA/cm^(2))and IPCE value(33.1%)of TiO_(2)-MOF-2 are about twice higher than that of pristine TiO_(2) due to the rich unsaturated sites of Ni-MOF.Meanwhile,the saturated coordination has caused the decline of PEC performance because of the obvious steric hindrance.Therefore,this work presents an insight for the effect of coordination state on PEC activity especially in MOF system.