The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contribu...The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contributing to addressing sustainability challenges.The S-scheme charge transfer mechanism enhances charge separation by maintaining strong redox potentials at both ends,facilitating both oxidation and reduction reactions.Herein,we synthesize a visible-light-responsive oxygen vacancy-rich In_(2)O_(3-x)/tubular carbon nitride(IO_(OV)/TCN)S-scheme heterojunction photocatalyst via electrostatic adherence for selec-tive 5-hydroxymethylfurfural(HMF)oxidation to 2,5-diformylfuran(DFF)and 2,5-furandicarboxylic acid(FDCA),alongside H_(2)production.Under anaerobic conditions and visible-light irradiation,the optimal IOOV/TCN-10 catalyst achieves an HMF conversion of 94.8%with a selectivity of 53.6%for DFF and FDCA,and a H_(2)yield of 754.05μmol g^(−1)in 3 h.The significantly improved photocatalytic activity results from enhanced visible-light absorption,reduced carrier recombination,and abundant catalytic active sites due to the synergistic effect of surface oxygen vacancies,the hollow nanotube-based architecture,and the S-scheme charge transfer mechanism.This work highlights the great potentials of S-scheme heterojunctions in biomass conversion for sustainable energy use and chemical production.展开更多
In this work,the TiO_(2)/Sb_(2)S_(3) nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC...In this work,the TiO_(2)/Sb_(2)S_(3) nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC activity of TiO_(2)/Sb_(2)S_(3) composite sample was investigated by electrochemical impedance analysis,including Nyquist and Mott-Schottky(M-S)plots.It was demonstrated that vacuum annealing could crystallize Sb_(2)S_(3) component and change its color from red to black,leading to an increment of photocurrent density from 1.9 A/m^(2) to 4.25 A/m^(2) at 0 V versus saturated calomel electrode(VSCE).The enhanced PEC performance was mainly attributed to the improved visible light absorption.Moreover,annealing treatment facilitated retarding the electron-hole recombination occurred at the solid/liquid interfaces.Our work might provide a novel strategy for enhancing the PEC performance of a semiconductor electrode.展开更多
V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for N...V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.展开更多
基金financially supported by the Natural Science Foundation of China(Nos.21972058,22102064,and 22302080)Anhui Key Laboratory of Nanomaterials and Nanotechnology,the Major Science and Technology Projects in Anhui Province(No.202305a12020006).
文摘The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contributing to addressing sustainability challenges.The S-scheme charge transfer mechanism enhances charge separation by maintaining strong redox potentials at both ends,facilitating both oxidation and reduction reactions.Herein,we synthesize a visible-light-responsive oxygen vacancy-rich In_(2)O_(3-x)/tubular carbon nitride(IO_(OV)/TCN)S-scheme heterojunction photocatalyst via electrostatic adherence for selec-tive 5-hydroxymethylfurfural(HMF)oxidation to 2,5-diformylfuran(DFF)and 2,5-furandicarboxylic acid(FDCA),alongside H_(2)production.Under anaerobic conditions and visible-light irradiation,the optimal IOOV/TCN-10 catalyst achieves an HMF conversion of 94.8%with a selectivity of 53.6%for DFF and FDCA,and a H_(2)yield of 754.05μmol g^(−1)in 3 h.The significantly improved photocatalytic activity results from enhanced visible-light absorption,reduced carrier recombination,and abundant catalytic active sites due to the synergistic effect of surface oxygen vacancies,the hollow nanotube-based architecture,and the S-scheme charge transfer mechanism.This work highlights the great potentials of S-scheme heterojunctions in biomass conversion for sustainable energy use and chemical production.
基金supported by the Fundamental Research Funds for the Central Universities(No.2019ZDPY04).
文摘In this work,the TiO_(2)/Sb_(2)S_(3) nanorod arrays(NRAs)were synthesized through a two-stage hydrothermal route for photoelectrochemical(PEC)water splitting.The effect of annealing treatment in Ar ambience on the PEC activity of TiO_(2)/Sb_(2)S_(3) composite sample was investigated by electrochemical impedance analysis,including Nyquist and Mott-Schottky(M-S)plots.It was demonstrated that vacuum annealing could crystallize Sb_(2)S_(3) component and change its color from red to black,leading to an increment of photocurrent density from 1.9 A/m^(2) to 4.25 A/m^(2) at 0 V versus saturated calomel electrode(VSCE).The enhanced PEC performance was mainly attributed to the improved visible light absorption.Moreover,annealing treatment facilitated retarding the electron-hole recombination occurred at the solid/liquid interfaces.Our work might provide a novel strategy for enhancing the PEC performance of a semiconductor electrode.
基金supported by the National Natural Science Foundation of China (51372137)the National High Technology Research and Development Program of China (863 Program,2015AA034603)~~
文摘V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.
