A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3(NH3-SCR) was determined.The effects of SO2 and H2O,and the...A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3(NH3-SCR) was determined.The effects of SO2 and H2O,and their combined effect,on the activity were examined at 340 ℃ for 24 h.The catalysts were characterized using N2 adsorption-desorption,X-ray diffraction,X-ray photoelectron spectroscopy,temperature-programmed reduction of H2(H2-TPR),temperature-programmed desorption of NH3(NH3-TPD),and in situ diffuse-reflectance infrared Fourier-transform spectroscopy(DRIFTS).The CuSO4/TiO2 catalysts had good activities,with low production of N2O above 340 ℃.SO2 or a combination of SO2 and H2O had little effect on the activity,and H2O caused only a slight decrease in activity during the experimental period.The NH3-TPD and H2-TPR results showed that CuSO4 increased the amounts of acid sites and adsorbed oxygen on the catalyst.In situ DRIFTS showed that the NH3-SCR reaction on the CuSO4/TiO2 catalysts followed an Eley-Rideal mechanism.The reaction of gaseous NO with NH3 adsorbed on Lewis acid sites to form N2 and H2O could be the main reaction pathway,and oxygen adsorption might favor this process.展开更多
With growing demand for propylene and increasing production of propane from shale gas,the technologies of propylene production,including direct dehydrogenation and oxidative dehydrogenation of propane,have drawn great...With growing demand for propylene and increasing production of propane from shale gas,the technologies of propylene production,including direct dehydrogenation and oxidative dehydrogenation of propane,have drawn great attention in recent years.In particular,direct dehydrogenation of propane to propylene is regarded as one of the most promising methods of propylene production because it is an on-purpose technique that exclusively yields propylene instead of a mixture of products.In this critical review,we provide the current investigations on the heterogeneous catalysts(such as Pt,CrOx,VOx,GaOx-based catalysts,and nanocarbons)used in the direct dehydrogenation of propane to propylene.A detailed comparison and discussion of the active sites,catalytic mechanisms,influencing factors(such as the structures,dispersions,and reducibilities of the catalysts and promoters),and supports for different types of catalysts is presented.Furthermore,rational designs and preparation of high-performance catalysts for propane dehydrogenation are proposed and discussed.展开更多
Applying quantitative temporal analysis of products reactor measurements, we studied the reactive removal of active oxygen present on Au/TiO2 catalysts after calcination at elevated temperatures (400 °C) by CO...Applying quantitative temporal analysis of products reactor measurements, we studied the reactive removal of active oxygen present on Au/TiO2 catalysts after calcination at elevated temperatures (400 °C) by CO pulses and its replenishment by O2 pulses at 80 °C, focusing on the nature of the active oxygen species. In contrast to previous studies, which mainly focused on and clarified the nature of the active oxygen species for the catalytic CO oxidation, which is reversibly formed and replenished under typical reaction conditions, this study demonstrates that directly after calcina‐tion an additional oxygen species is present. This species is also active for the CO oxidation, but it is not or only very little formed under typical reaction conditions. Implications of these results on the mechanistic understanding of the CO oxidation on Au/TiO2, in particular on the role of different active oxygen species, will be discussed.展开更多
Atomic energy is an important part of current energy resources.Production of nuclear weapons and applications of nuclear fuels in nuclear power plants have accumulated numerous spent fuels containing238U compounds,whi...Atomic energy is an important part of current energy resources.Production of nuclear weapons and applications of nuclear fuels in nuclear power plants have accumulated numerous spent fuels containing238U compounds,which are critical nuclear materials.How to reduce the nuclear wastes and to make use of the spent uranium are key scientific issues of environmental and nuclear science.We have reviewed here the physiochemical properties and photocatalytic mechanisms of homogeneous and heterogeneous uranium-containing materials.The current research efforts demonstrate that spent fuels can become promising new photocatalytic materials.展开更多
基金supported by the Bureau of Science and Technology,Fujian Province,China(2015H0043)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB05050500)the National Natural Science Foundation of China(21403210)~~
文摘A series of CuSO4/TiO2 catalysts were prepared using a wet impregnation method.The activity of each sample in the selective catalytic reduction of NO by NH3(NH3-SCR) was determined.The effects of SO2 and H2O,and their combined effect,on the activity were examined at 340 ℃ for 24 h.The catalysts were characterized using N2 adsorption-desorption,X-ray diffraction,X-ray photoelectron spectroscopy,temperature-programmed reduction of H2(H2-TPR),temperature-programmed desorption of NH3(NH3-TPD),and in situ diffuse-reflectance infrared Fourier-transform spectroscopy(DRIFTS).The CuSO4/TiO2 catalysts had good activities,with low production of N2O above 340 ℃.SO2 or a combination of SO2 and H2O had little effect on the activity,and H2O caused only a slight decrease in activity during the experimental period.The NH3-TPD and H2-TPR results showed that CuSO4 increased the amounts of acid sites and adsorbed oxygen on the catalyst.In situ DRIFTS showed that the NH3-SCR reaction on the CuSO4/TiO2 catalysts followed an Eley-Rideal mechanism.The reaction of gaseous NO with NH3 adsorbed on Lewis acid sites to form N2 and H2O could be the main reaction pathway,and oxygen adsorption might favor this process.
基金supported by the National Natural Science Foundation of China(21421001,21573115)the Fundamental Research Funds for the Central Universities(63185015)the Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering(2017-K13)~~
文摘With growing demand for propylene and increasing production of propane from shale gas,the technologies of propylene production,including direct dehydrogenation and oxidative dehydrogenation of propane,have drawn great attention in recent years.In particular,direct dehydrogenation of propane to propylene is regarded as one of the most promising methods of propylene production because it is an on-purpose technique that exclusively yields propylene instead of a mixture of products.In this critical review,we provide the current investigations on the heterogeneous catalysts(such as Pt,CrOx,VOx,GaOx-based catalysts,and nanocarbons)used in the direct dehydrogenation of propane to propylene.A detailed comparison and discussion of the active sites,catalytic mechanisms,influencing factors(such as the structures,dispersions,and reducibilities of the catalysts and promoters),and supports for different types of catalysts is presented.Furthermore,rational designs and preparation of high-performance catalysts for propane dehydrogenation are proposed and discussed.
文摘Applying quantitative temporal analysis of products reactor measurements, we studied the reactive removal of active oxygen present on Au/TiO2 catalysts after calcination at elevated temperatures (400 °C) by CO pulses and its replenishment by O2 pulses at 80 °C, focusing on the nature of the active oxygen species. In contrast to previous studies, which mainly focused on and clarified the nature of the active oxygen species for the catalytic CO oxidation, which is reversibly formed and replenished under typical reaction conditions, this study demonstrates that directly after calcina‐tion an additional oxygen species is present. This species is also active for the CO oxidation, but it is not or only very little formed under typical reaction conditions. Implications of these results on the mechanistic understanding of the CO oxidation on Au/TiO2, in particular on the role of different active oxygen species, will be discussed.
基金supported by the National Basic Research Program of China(973 Project,2011CB932400)Strategic International Collaborative Research Program of China(SICORP,2013DFG50150)
文摘Atomic energy is an important part of current energy resources.Production of nuclear weapons and applications of nuclear fuels in nuclear power plants have accumulated numerous spent fuels containing238U compounds,which are critical nuclear materials.How to reduce the nuclear wastes and to make use of the spent uranium are key scientific issues of environmental and nuclear science.We have reviewed here the physiochemical properties and photocatalytic mechanisms of homogeneous and heterogeneous uranium-containing materials.The current research efforts demonstrate that spent fuels can become promising new photocatalytic materials.