A series of high surface area graphitic carbon materials （HSGCs） were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x （x is the ball-milling t...A series of high surface area graphitic carbon materials （HSGCs） were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x （x is the ball-milling time in hour） catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.展开更多
Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by ...Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by microwave-assisted polyol process. The physical and electrochemical properties of the catalysts were characterized by X-ray diffraction （XRD）, transmission electron microscope （TEM）, CO stripping voltammetry, cyclic voltammetry （CV） and chronoamperometry （CA）. The results showed that the Nation incorporation in CNTs-Nation composites did not significantly alter the oxygen-containing groups on the CNTs surface. The Pt-Ru catalyst supported on CNTs-Nafion composites with 2 wt% Naton showed good dispersion and the best CO oxidation and methanol electro-oxidation activities.展开更多
A series of 3 wt% Ru embedded on ordered mesoporous carbon （OMC） catalysts with different pore sizes were prepared by autoreduction between ruthenium precursors and carbon sources at 1123 K. Ru nanoparticles were em...A series of 3 wt% Ru embedded on ordered mesoporous carbon （OMC） catalysts with different pore sizes were prepared by autoreduction between ruthenium precursors and carbon sources at 1123 K. Ru nanoparticles were embedded on the carbon walls of OMC. Characterization technologies including power X-ray diffraction （XRD）, nitrogen adsorption-desorption, transmission electron microscopy （TEM）, and hydrogen temperature-programmed reduction （H2-TPR） were used to scrutinize the catalysts. The catalyst activity for Fischer-Tropsch synthesis （FTS） was measured in a fixed bed reactor. It was revealed that 3 wt% Ru-OMC catalysts exhibited highly ordered mesoporous structure and large surface area. Compared with the catalysts with smaller pores, the catalysts with larger pores were inclined to form larger Ru particles. These 3 wt% Ru-OMC catalysts with different pore sizes were more stable than 3 wt% Ru/AC catalyst during the FTS reactions because Ru particles were embedded on the carbon walls, suppressing particles aggregation, movement and oxidation. The catalytic activity and C5＋ selectivity were found to increase with the increasing pore size, however, CH4 selectivity showed the opposite trend. These changes may be explained in terms of the special environment of the active Ru sites and the diffusion of products in the pores of the catalysts, suggesting that the activity and hydrocarbon selectivity are more dependent on the pore size of OMC than on the Ru particle size.展开更多
In this work, CO_2 methanation has been investigated over Ru-based catalysts.The effects of promoters on the activity, selectivity and reduction properties of the Ru/sepiolitecatalyst were analyzed by kinetic and ther...In this work, CO_2 methanation has been investigated over Ru-based catalysts.The effects of promoters on the activity, selectivity and reduction properties of the Ru/sepiolitecatalyst were analyzed by kinetic and thermodynamic methods. The catalysts were characterized bymeans of TPD, and the results revealed that the addition of Mo, Mn or Co improved the properties ofthe Ru/sepiolite catalyst. The effects of promoters could affect the change of enthalpy, entropy andchemical potential.展开更多
Behaviour of excited Ru(bpy)2+3 bound to the surface of water-soluble single-walled carbon nanotubes on addition of other cations have been investigated by measuring Ru(bpy) luminescence. In contrast to what was obser...Behaviour of excited Ru(bpy)2+3 bound to the surface of water-soluble single-walled carbon nanotubes on addition of other cations have been investigated by measuring Ru(bpy) luminescence. In contrast to what was observed with a solution containing rod-like aggregation particles of Nafion, we found that Ru(bpy)2+3 has a stronger attraction than that of other cations to the sulfonic groups on the carbon nanotubes. Such a difference is attributed to the unique micro-environmental characteristics of the molecular assemblies.展开更多
Carbon nanotubes （CNTs） supported Pt-Ru and Pt-Ru-Ni catalysts were prepared by chemical reduction of metal precursors with sodium borohydride at room temperature. The crystallographic properties and composition of ...Carbon nanotubes （CNTs） supported Pt-Ru and Pt-Ru-Ni catalysts were prepared by chemical reduction of metal precursors with sodium borohydride at room temperature. The crystallographic properties and composition of the catalysts were characterized by X-ray diffraction （XRD） and energy dispersive X-ray （EDX） analysis, and the catalytic activity and stability for methanol electro-oxidation were measured by electrochemical impedance spectroscopy （EIS）, linear sweep voltammetries （LSV）, and chronoamperometry （CA）. The results show that the catalysts exhibit face-centered cubic （fcc） structure. The particle size of Pt-Ru-Ni/CNTs catalyst is about 4.8 nm. The catalytic activity and stability of the Pt-Ru-Ni/CNTs catalyst are higher than those of Pt-Ru/CNTs catalyst.展开更多
Molecular nitrogen is relatively inert and the activation of its triple bond is full of challenges and of significance.Hence,searching for an efficiently heterogeneous catalyst with high stability and dispersion is on...Molecular nitrogen is relatively inert and the activation of its triple bond is full of challenges and of significance.Hence,searching for an efficiently heterogeneous catalyst with high stability and dispersion is one of the important targets of chemical technology.Here,we report a Ba‐K/Ru‐MC catalyst with Ru particle size of 1.5–2.5 nm semi‐embedded in a mesoporous C matrix and with dual promoters of Ba and K that exhibits a higher activity than the supported Ba‐Ru‐K/MC catalyst,although both have similar metal particle sizes for ammonia synthesis.Further,the Ba‐K/Ru‐MC catalyst is more active than commercial fused Fe catalysts and supported Ru catalysts.Characterization techniques such as high‐resolution transmission electron microscopy,N2 physisorption,CO chemisorption,and temperature‐programmed reduction suggest that the Ru nanoparticles have strong interactions with the C matrix in Ba‐K/Ru‐MC,which may facilitate electron transport better than supported nanoparticles.展开更多
The mechanism of CO 2 methanation over Ru/ZrO 2 catalyst has been studied by means of diffuse reflectance infrared Fourier-transform spectroscopy. The results indicate that the formation of carbon-containing species o...The mechanism of CO 2 methanation over Ru/ZrO 2 catalyst has been studied by means of diffuse reflectance infrared Fourier-transform spectroscopy. The results indicate that the formation of carbon-containing species on the surface of catalyst is involved in the catalytic process. The adsorbed carbonate, formate and carbon monoxide can be detected on the surface of Ru/ZrO 2 catalyst. The surface carbonate and formate are much more abundant than the surface carbon monoxide. The surface carbonate and formate are main intermediates for the catalytic methanation of CO 2 over Ru/ZrO 2 catalyst, which can be directly hydrogenated to methane in the presence of hydrogen.展开更多
基金supported by the Natural Science Foundation of China(NSFC Grant No.20803064)the Natural Science Foundation of Zhejiang Provence(Y4090348 and LY12B03007)Qianjiang Talent Project in Zhejiang Province(2010R10039 and 2013R10056)
文摘A series of high surface area graphitic carbon materials （HSGCs） were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x （x is the ball-milling time in hour） catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.
基金supported by National Natural Science Foundation of China (NO.0576023)Key Project of Science and Technology Department of Guangdong Province (NO.2008B010800036 NO.2008B010800037)
文摘Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by microwave-assisted polyol process. The physical and electrochemical properties of the catalysts were characterized by X-ray diffraction （XRD）, transmission electron microscope （TEM）, CO stripping voltammetry, cyclic voltammetry （CV） and chronoamperometry （CA）. The results showed that the Nation incorporation in CNTs-Nation composites did not significantly alter the oxygen-containing groups on the CNTs surface. The Pt-Ru catalyst supported on CNTs-Nafion composites with 2 wt% Naton showed good dispersion and the best CO oxidation and methanol electro-oxidation activities.
基金supported by the National Natural Science Foundation of China (Grant No. 21073238)the National Basic Research Program of China (Grant No. 2011CB211704)
文摘A series of 3 wt% Ru embedded on ordered mesoporous carbon （OMC） catalysts with different pore sizes were prepared by autoreduction between ruthenium precursors and carbon sources at 1123 K. Ru nanoparticles were embedded on the carbon walls of OMC. Characterization technologies including power X-ray diffraction （XRD）, nitrogen adsorption-desorption, transmission electron microscopy （TEM）, and hydrogen temperature-programmed reduction （H2-TPR） were used to scrutinize the catalysts. The catalyst activity for Fischer-Tropsch synthesis （FTS） was measured in a fixed bed reactor. It was revealed that 3 wt% Ru-OMC catalysts exhibited highly ordered mesoporous structure and large surface area. Compared with the catalysts with smaller pores, the catalysts with larger pores were inclined to form larger Ru particles. These 3 wt% Ru-OMC catalysts with different pore sizes were more stable than 3 wt% Ru/AC catalyst during the FTS reactions because Ru particles were embedded on the carbon walls, suppressing particles aggregation, movement and oxidation. The catalytic activity and C5＋ selectivity were found to increase with the increasing pore size, however, CH4 selectivity showed the opposite trend. These changes may be explained in terms of the special environment of the active Ru sites and the diffusion of products in the pores of the catalysts, suggesting that the activity and hydrocarbon selectivity are more dependent on the pore size of OMC than on the Ru particle size.
基金Project supported by the National Natural Science Foundation of China
文摘In this work, CO_2 methanation has been investigated over Ru-based catalysts.The effects of promoters on the activity, selectivity and reduction properties of the Ru/sepiolitecatalyst were analyzed by kinetic and thermodynamic methods. The catalysts were characterized bymeans of TPD, and the results revealed that the addition of Mo, Mn or Co improved the properties ofthe Ru/sepiolite catalyst. The effects of promoters could affect the change of enthalpy, entropy andchemical potential.
文摘Behaviour of excited Ru(bpy)2+3 bound to the surface of water-soluble single-walled carbon nanotubes on addition of other cations have been investigated by measuring Ru(bpy) luminescence. In contrast to what was observed with a solution containing rod-like aggregation particles of Nafion, we found that Ru(bpy)2+3 has a stronger attraction than that of other cations to the sulfonic groups on the carbon nanotubes. Such a difference is attributed to the unique micro-environmental characteristics of the molecular assemblies.
基金The project is supported by the National Natural Science Foundation of China (20576023)the Science and Technology Project of Guangzhou City (2005 J1-C0361)the Key Project of Education Bureau of Guangzhou City (2052).
文摘Carbon nanotubes （CNTs） supported Pt-Ru and Pt-Ru-Ni catalysts were prepared by chemical reduction of metal precursors with sodium borohydride at room temperature. The crystallographic properties and composition of the catalysts were characterized by X-ray diffraction （XRD） and energy dispersive X-ray （EDX） analysis, and the catalytic activity and stability for methanol electro-oxidation were measured by electrochemical impedance spectroscopy （EIS）, linear sweep voltammetries （LSV）, and chronoamperometry （CA）. The results show that the catalysts exhibit face-centered cubic （fcc） structure. The particle size of Pt-Ru-Ni/CNTs catalyst is about 4.8 nm. The catalytic activity and stability of the Pt-Ru-Ni/CNTs catalyst are higher than those of Pt-Ru/CNTs catalyst.
基金supported by the National Natural Science Foundation of China(20803064)the Natural Science Foundation of Zhejiang Provence(LY17B030010)~~
文摘Molecular nitrogen is relatively inert and the activation of its triple bond is full of challenges and of significance.Hence,searching for an efficiently heterogeneous catalyst with high stability and dispersion is one of the important targets of chemical technology.Here,we report a Ba‐K/Ru‐MC catalyst with Ru particle size of 1.5–2.5 nm semi‐embedded in a mesoporous C matrix and with dual promoters of Ba and K that exhibits a higher activity than the supported Ba‐Ru‐K/MC catalyst,although both have similar metal particle sizes for ammonia synthesis.Further,the Ba‐K/Ru‐MC catalyst is more active than commercial fused Fe catalysts and supported Ru catalysts.Characterization techniques such as high‐resolution transmission electron microscopy,N2 physisorption,CO chemisorption,and temperature‐programmed reduction suggest that the Ru nanoparticles have strong interactions with the C matrix in Ba‐K/Ru‐MC,which may facilitate electron transport better than supported nanoparticles.
文摘The mechanism of CO 2 methanation over Ru/ZrO 2 catalyst has been studied by means of diffuse reflectance infrared Fourier-transform spectroscopy. The results indicate that the formation of carbon-containing species on the surface of catalyst is involved in the catalytic process. The adsorbed carbonate, formate and carbon monoxide can be detected on the surface of Ru/ZrO 2 catalyst. The surface carbonate and formate are much more abundant than the surface carbon monoxide. The surface carbonate and formate are main intermediates for the catalytic methanation of CO 2 over Ru/ZrO 2 catalyst, which can be directly hydrogenated to methane in the presence of hydrogen.
