Activated carbon (AC) supported silver catalysts were prepared by incipient wetness impregnation method and their catalytic performance for CO preferential oxidation (PROX) in excess H2 was evaluated. Ag/AC cataly...Activated carbon (AC) supported silver catalysts were prepared by incipient wetness impregnation method and their catalytic performance for CO preferential oxidation (PROX) in excess H2 was evaluated. Ag/AC catalysts, after reduction in H2 at low temperatures (≤200 ℃) following heat treatment in He at 200 ℃ (He200H200), exhibited the best catalytic properties. Temperature-programmed desorption (TPD), X-ray diffraction (XRD) and temperature-programmed reduction (TPR) results indicated that silver oxides were produced during heat treatment in He at 200 ℃ which were reduced to metal silver nanoparticles in H2 at low temperatures (≤200 ℃), simultaneously generating the adsorbed water/OH. CO conversion was enhanced 40% after water treatment following heat treatment in He at 600 ℃. These results imply that the metal silver nanoparticles are the active species and the adsorbed water/OH has noticeable promotion effects on CO oxidation. However, the promotion effect is still limited compared to gold catalysts under the similar conditions, which may be the reason of low selectivity to CO oxidation in PROX over silver catalysts. The reported Ag/AC-S-He catalyst after He200H200 treatment displayed similar PROX of CO reaction properties to Ag/SiO2. This means that Ag/AC catalyst is also an efficient low-temperature CO oxidation catalyst.展开更多
Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared usin...Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO_2 and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl_2 caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.展开更多
A new carbonaceous catalyst with sulfonic acid group (-SO3H) was prepared by incomplete carbonization of β-cyclodextrin followed by sulfonation.The sulfonated amorphous carbon was characterized by IR,elemental anal...A new carbonaceous catalyst with sulfonic acid group (-SO3H) was prepared by incomplete carbonization of β-cyclodextrin followed by sulfonation.The sulfonated amorphous carbon was characterized by IR,elemental analysis,DSC-TGA and PXRD,and the catalytic activity was investigated to be an efficient catalyst for the esterification reactions with maximum yield of 87%.The sulfonated carbonaceous catalyst was readily separated from the reaction solution and keeps approximately equal catalytic activity.The results confirm that the active centre is the hydrophilic sulfonic acid functional group in the esterification reactions.展开更多
基金supported by the National Natural Science Foundation of China (No. 21207039)the Natural Science Foundation of Guangdong Province, China (Grant No. S2011010000737)+2 种基金the Doctoral Fund of Ministry of Education of China (20110172120017)the Fundamental Research Funds for the Central Universities (Grant No. 2011zm 0048)the Key Laboratory of Renewable Energy and Gas Hydrate, Chinese Academy of Sciences (No. Y007K1)
文摘Activated carbon (AC) supported silver catalysts were prepared by incipient wetness impregnation method and their catalytic performance for CO preferential oxidation (PROX) in excess H2 was evaluated. Ag/AC catalysts, after reduction in H2 at low temperatures (≤200 ℃) following heat treatment in He at 200 ℃ (He200H200), exhibited the best catalytic properties. Temperature-programmed desorption (TPD), X-ray diffraction (XRD) and temperature-programmed reduction (TPR) results indicated that silver oxides were produced during heat treatment in He at 200 ℃ which were reduced to metal silver nanoparticles in H2 at low temperatures (≤200 ℃), simultaneously generating the adsorbed water/OH. CO conversion was enhanced 40% after water treatment following heat treatment in He at 600 ℃. These results imply that the metal silver nanoparticles are the active species and the adsorbed water/OH has noticeable promotion effects on CO oxidation. However, the promotion effect is still limited compared to gold catalysts under the similar conditions, which may be the reason of low selectivity to CO oxidation in PROX over silver catalysts. The reported Ag/AC-S-He catalyst after He200H200 treatment displayed similar PROX of CO reaction properties to Ag/SiO2. This means that Ag/AC catalyst is also an efficient low-temperature CO oxidation catalyst.
基金Supported by the National Science Fund for Excellent Young Scholars of China(No.51522405)
文摘Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO_2 and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl_2 caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.
基金Funded by the Guangdong Science Project (No.2008B011000015)
文摘A new carbonaceous catalyst with sulfonic acid group (-SO3H) was prepared by incomplete carbonization of β-cyclodextrin followed by sulfonation.The sulfonated amorphous carbon was characterized by IR,elemental analysis,DSC-TGA and PXRD,and the catalytic activity was investigated to be an efficient catalyst for the esterification reactions with maximum yield of 87%.The sulfonated carbonaceous catalyst was readily separated from the reaction solution and keeps approximately equal catalytic activity.The results confirm that the active centre is the hydrophilic sulfonic acid functional group in the esterification reactions.