The solar-driven photocatalytic technology has shown great potential in nitrate(NO_(3)^(-))pollutants reduction,however,it has been greatly hindered by the complex preparation and high cost of photocatalysts.Herein,a ...The solar-driven photocatalytic technology has shown great potential in nitrate(NO_(3)^(-))pollutants reduction,however,it has been greatly hindered by the complex preparation and high cost of photocatalysts.Herein,a relatively low-cost photocatalyst,rutile and anatase mixed phase TiO_(2) was synthesized by a facile microwave-hydrothermal method.Meanwhile,oxygen vacancy is successfully generated,leading to an acidic surface for strong adsorption towards NO_(3)^(-),which further improved the reduction activity.Compared with the commercial P25,a higher NO_(3)^(-) conversion of ca.100%and nitrogen(N_(2)) selectivity of 87%were achieved under UV(365 nm)irradiation within 2 h.This research provides a promising strategy for designing efficient noble metal free photocatalyst in the NO_(3)^(-) reduction.展开更多
Ammonia is one of the most essential chemicals in the modern society but its production still heavily relies on energy-consuming Haber-Bosch processes.The photocatalytic reduction of nitrogen with water for ammonia pr...Ammonia is one of the most essential chemicals in the modern society but its production still heavily relies on energy-consuming Haber-Bosch processes.The photocatalytic reduction of nitrogen with water for ammonia production has attracted much attention recently due to its synthesis under mild conditions at room temperature and atmospheric pressure using sunlight.Herein,we report a high-performance Au/MIL-100(Cr)photocatalyst,comprising MIL-100(Cr)and Au nanoparticles in photocatalytic nitrogen reduction to ammonia at ambient conditions under visible light irradiation.The optimized photocatalyst(i.e.,0.10Au/MIL-100(Cr))achieved the excellent ammonia production rate with 39.9μg g_(cat)^(-1) h^(-1) compared with pure MIL-100(Cr)(2.73μg gcat^(-1) h^(-1)),which was nearly 15 times that on pure MIL-100(Cr).The remarkable activity could be attributed to the adsorption-plasmonic synergistic effects in which the MIL-100(Cr)and Au are responsible to the strong trapping and adsorption of N2 molecules and photo-induced plasmonic hot electrons activating and decomposing the N2 molecules,respectively.This study might provide a new strategy for designing an efficient plasmonic photocatalyst to improve the photocatalytic performance of N2 fixation under visible light irradiation.展开更多
基金supported by the National Key Research and Development Program of China(No.2020YFA0211004)and National Natural Science Foundation of China(Nos.21876112,21876113,22022608,92034301)+2 种基金“111”Innovation and Talent Recruitment Base on Photochemical and Energy Materials(No.D18020)Ministry of Education,and Shanghai Key Laboratory of Rare Earth Functional Materials,Shanghai Engineering Research Center of Green Energy Chemical Engineering(Nos.18DZ2254200)Shanghai government(Nos.18SG41,309-AC9103-21-413002,19YF1436600)。
文摘The solar-driven photocatalytic technology has shown great potential in nitrate(NO_(3)^(-))pollutants reduction,however,it has been greatly hindered by the complex preparation and high cost of photocatalysts.Herein,a relatively low-cost photocatalyst,rutile and anatase mixed phase TiO_(2) was synthesized by a facile microwave-hydrothermal method.Meanwhile,oxygen vacancy is successfully generated,leading to an acidic surface for strong adsorption towards NO_(3)^(-),which further improved the reduction activity.Compared with the commercial P25,a higher NO_(3)^(-) conversion of ca.100%and nitrogen(N_(2)) selectivity of 87%were achieved under UV(365 nm)irradiation within 2 h.This research provides a promising strategy for designing efficient noble metal free photocatalyst in the NO_(3)^(-) reduction.
基金supported by the National Natural Science Foundation of China(Nos.21876112,21876113,21261140333,22022608 and 92034301)Shanghai Pujiang Program(No.20PJ1411800)+3 种基金the National Key Research and Development Program of China(No.2020YFA0211004)"111"Innovation and Talent Recruitment Base on Photochemical and Energy Materials(No.D18020)Ministry of Education,and Shanghai Key Laboratory of Rare Earth Functional Materials,Shanghai Engineering Research Center of Green Energy Chemical Engineering(No.18DZ2254200)Shanghai government(Nos.18SG41,309-AC9103-21-413002).
文摘Ammonia is one of the most essential chemicals in the modern society but its production still heavily relies on energy-consuming Haber-Bosch processes.The photocatalytic reduction of nitrogen with water for ammonia production has attracted much attention recently due to its synthesis under mild conditions at room temperature and atmospheric pressure using sunlight.Herein,we report a high-performance Au/MIL-100(Cr)photocatalyst,comprising MIL-100(Cr)and Au nanoparticles in photocatalytic nitrogen reduction to ammonia at ambient conditions under visible light irradiation.The optimized photocatalyst(i.e.,0.10Au/MIL-100(Cr))achieved the excellent ammonia production rate with 39.9μg g_(cat)^(-1) h^(-1) compared with pure MIL-100(Cr)(2.73μg gcat^(-1) h^(-1)),which was nearly 15 times that on pure MIL-100(Cr).The remarkable activity could be attributed to the adsorption-plasmonic synergistic effects in which the MIL-100(Cr)and Au are responsible to the strong trapping and adsorption of N2 molecules and photo-induced plasmonic hot electrons activating and decomposing the N2 molecules,respectively.This study might provide a new strategy for designing an efficient plasmonic photocatalyst to improve the photocatalytic performance of N2 fixation under visible light irradiation.