The selective catalytic oxidation of toluene with hydrogen peroxide over V-Mo-based catalysts under mild conditions was studied.The promotion effect of Mo on the catalysts was studied with V/Al2O3 and Mo/Al2O3 as refe...The selective catalytic oxidation of toluene with hydrogen peroxide over V-Mo-based catalysts under mild conditions was studied.The promotion effect of Mo on the catalysts was studied with V/Al2O3 and Mo/Al2O3 as reference samples.The catalysts were characterized by XRD,TPR,and XPS techniques.The results show that the addition of Mo to V/Al2O3 may change the distribution of V species on Al2O3 surface.Over V-Mo/Al2O3 catalyst,highly dispersed amorphous V species facilitates benzaldehyde formation,and crystalline V2O5 species increases the conversion of toluene but decreases the selectivity to benzaldehyde,while AlVMoO7 species favors both the conversion of toluene and the formation of cresols.The yield of benzaldehyde depends remarkably on the surface O/Al and Mo/V atomic ratios,and gets to a maximum value of 13.2% with a selectivity of 79.5% at an O/Al atomic ratio of 3.0 and Mo/V atomic ratio of 0.7.展开更多
The key issues to improve the performance of photocatalysts for selective oxidation of toluene are promoting the migration and separation of charge carrier,and enhancing the generation of active oxygen species.It is k...The key issues to improve the performance of photocatalysts for selective oxidation of toluene are promoting the migration and separation of charge carrier,and enhancing the generation of active oxygen species.It is known that the construction of compact heterojunction is an efficient protocol to inhibit photogenerated electron-hole recombination.In this work,a 2D-2D[Bi_(6)O_(6)(OH)_(3)](NO_(3))3·1.5H2O-Bi_(2)MoO_(6)(denoted as BBN-BMO)composite heterojunction has been prepared by one-step hydrothermal method for the first time.The tetragonal phase BBN in the composite plays the role of transferring electrons from the visible light activated orthorhombic phase BMO and promoting the generation of active·O_(2)^(-),the holes left in BMO are used to activate toluene and produce benzyl radical,thus greatly improving the photocatalytic performance for selective oxidation of toluene.The toluene conversion rate of BBN-BMO is 3466μmol·g^(-1)·h^(-1),which is three times that of pure BMO.The selectivity to benzalde-hyde is 94.2%.In addition,reasonable mechanism has been speculated based on a series of control experiments.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.20502017and20072024)the Teaching and ResearchAward Program for Outstanding Young Teachers in Higher Education Institutions of Ministry of Education,Chinathe ScienceFoundation for Young Teachers of Sichuan University.
文摘The selective catalytic oxidation of toluene with hydrogen peroxide over V-Mo-based catalysts under mild conditions was studied.The promotion effect of Mo on the catalysts was studied with V/Al2O3 and Mo/Al2O3 as reference samples.The catalysts were characterized by XRD,TPR,and XPS techniques.The results show that the addition of Mo to V/Al2O3 may change the distribution of V species on Al2O3 surface.Over V-Mo/Al2O3 catalyst,highly dispersed amorphous V species facilitates benzaldehyde formation,and crystalline V2O5 species increases the conversion of toluene but decreases the selectivity to benzaldehyde,while AlVMoO7 species favors both the conversion of toluene and the formation of cresols.The yield of benzaldehyde depends remarkably on the surface O/Al and Mo/V atomic ratios,and gets to a maximum value of 13.2% with a selectivity of 79.5% at an O/Al atomic ratio of 3.0 and Mo/V atomic ratio of 0.7.
基金National Natural Science Foundation of China(Nos.21975069,21725602,22108067,and 21938002)Innovative Research Groups of Hunan Province(No.2019JJ10001)Science and Technology Planning Project of Hunan Province(No.2019RS3010).
文摘The key issues to improve the performance of photocatalysts for selective oxidation of toluene are promoting the migration and separation of charge carrier,and enhancing the generation of active oxygen species.It is known that the construction of compact heterojunction is an efficient protocol to inhibit photogenerated electron-hole recombination.In this work,a 2D-2D[Bi_(6)O_(6)(OH)_(3)](NO_(3))3·1.5H2O-Bi_(2)MoO_(6)(denoted as BBN-BMO)composite heterojunction has been prepared by one-step hydrothermal method for the first time.The tetragonal phase BBN in the composite plays the role of transferring electrons from the visible light activated orthorhombic phase BMO and promoting the generation of active·O_(2)^(-),the holes left in BMO are used to activate toluene and produce benzyl radical,thus greatly improving the photocatalytic performance for selective oxidation of toluene.The toluene conversion rate of BBN-BMO is 3466μmol·g^(-1)·h^(-1),which is three times that of pure BMO.The selectivity to benzalde-hyde is 94.2%.In addition,reasonable mechanism has been speculated based on a series of control experiments.