Au]Cel_xZrxO2 catalysts （x = 0-0.8） were prepared by a deposition-precipitation method using Cel_xZrxO2 nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentar...Au]Cel_xZrxO2 catalysts （x = 0-0.8） were prepared by a deposition-precipitation method using Cel_xZrxO2 nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentary means such as X-ray diffraction, Raman, scanning trans- mission electron microscopy and X-ray photoelectron spectroscopy （XPS）. These Au catalysts possessed similar sizes and crystalline phases of Cel_xZrzO2 supports as well as similar sizes and oxidation states of Au nanoparticles. The oxidation state of Au nanoparticles was dominated by Au~ especially in CO oxidation. Their activities were examined in CO oxidation at different temperatures in the range of 303-333 K. The CO oxidation rates normalized per Au atoms increased with the increasing Ce contents, and reached the maximum value over Au/CeO2. Such change was in parallel with the change in the oxygen storage capacity values, i.e. the amounts of active oxygen species on Au/Cel_zZrzO2 catalysts. The excellent correlation between the two properties of the catalysts suggests that the intrinsic support effects on the CO oxidation rates is related to the effects on the adsorption and activation of O2 on Au/Cel_xZrxO2 catalysts. Such understanding on the support effects may be useful for designing more active Au catalysts, for example, by tuning the redox properties of oxide supports.展开更多
The effect of support calcination temperature on the benzene selective hydrogenation performance of the Ru-Ce-B/ZrO2 catalysts was investigated.It was found that with increasing calcination temperature,the surface are...The effect of support calcination temperature on the benzene selective hydrogenation performance of the Ru-Ce-B/ZrO2 catalysts was investigated.It was found that with increasing calcination temperature,the surface area decreased,on the contrary,the pore size and the amount of monoclinic phase increased.With increasing support calcination temperature,the activity of the catalyst roughly decreased and cyclohexene selectivity increased.The activity decreased due to the decrease of the surface areas.The increase of the cyclohexene selectivity was correlated not only with the decrease of the surface areas but also with the increase of monoclinic phases,rich in surface hydroxyl,and the enlarged pore size of zirconia.This suggests the monoclinic zirconia with a medium surface area,rather than a big one,and a mesoporous structure,even including some macropores,is an ideal support of the catalyst for benzene selective hydrogenation.展开更多
基金the National Natural Science Foundation of China(20825310,20973011)the National Basic Research Program of China(973 Program,2011CB201400,2011CB808700)
文摘Au]Cel_xZrxO2 catalysts （x = 0-0.8） were prepared by a deposition-precipitation method using Cel_xZrxO2 nanoparticles as supports with variable Ce and Zr contents. Their structures were characterized by complimentary means such as X-ray diffraction, Raman, scanning trans- mission electron microscopy and X-ray photoelectron spectroscopy （XPS）. These Au catalysts possessed similar sizes and crystalline phases of Cel_xZrzO2 supports as well as similar sizes and oxidation states of Au nanoparticles. The oxidation state of Au nanoparticles was dominated by Au~ especially in CO oxidation. Their activities were examined in CO oxidation at different temperatures in the range of 303-333 K. The CO oxidation rates normalized per Au atoms increased with the increasing Ce contents, and reached the maximum value over Au/CeO2. Such change was in parallel with the change in the oxygen storage capacity values, i.e. the amounts of active oxygen species on Au/Cel_zZrzO2 catalysts. The excellent correlation between the two properties of the catalysts suggests that the intrinsic support effects on the CO oxidation rates is related to the effects on the adsorption and activation of O2 on Au/Cel_xZrxO2 catalysts. Such understanding on the support effects may be useful for designing more active Au catalysts, for example, by tuning the redox properties of oxide supports.
文摘The effect of support calcination temperature on the benzene selective hydrogenation performance of the Ru-Ce-B/ZrO2 catalysts was investigated.It was found that with increasing calcination temperature,the surface area decreased,on the contrary,the pore size and the amount of monoclinic phase increased.With increasing support calcination temperature,the activity of the catalyst roughly decreased and cyclohexene selectivity increased.The activity decreased due to the decrease of the surface areas.The increase of the cyclohexene selectivity was correlated not only with the decrease of the surface areas but also with the increase of monoclinic phases,rich in surface hydroxyl,and the enlarged pore size of zirconia.This suggests the monoclinic zirconia with a medium surface area,rather than a big one,and a mesoporous structure,even including some macropores,is an ideal support of the catalyst for benzene selective hydrogenation.
