Ten kinds of activated carbon from different raw materials were used as supports to prepare ruthenium catalysts. N_2 physisorption and CO chemisorption were carried out to investigate the pore size distribution and th...Ten kinds of activated carbon from different raw materials were used as supports to prepare ruthenium catalysts. N_2 physisorption and CO chemisorption were carried out to investigate the pore size distribution and the ruthenium dispersion of the catalysts. It was found that the Ru dispersion of the catalyst was closely related to not only the texture of carbon support but also the purity of activated carbon. The activities of a series of the carbon-supported barium-promoted Ru catalysts for ammonia synthesis were measured at 425 ℃, 10 0 MPa and 10 000 h -1. The result shows that the same raw material activated carbon, with a high purity, high surface area, large pore volume and reasonable pore size distribution might disperse ruthenium and promoter sufficiently, which activated carbon as support, could be used to manufacture ruthenium catalyst with a high activity for ammonia synthesis. The different raw material activated carbon as the support would greatly influence the catalytic properties of the ruthenium catalyst for ammonia synthesis. For example, with coconut shell carbon(AC1) as the support, the ammonia concentration in the effluent was 13 17% over 4%Ru-BaO/AC1 catalyst, while with the desulfurized coal carbon(AC10) as the support, that in the effluent was only 1 37% over 4%Ru-BaO/AC10 catalyst.展开更多
Suzuki-Miyaura reaction of aryl halides with phenylboronic acid using a heterogeneous palladium catalyst based on activated carbons(AC) was systematically investigated in this work. Two different reaction modes(batch ...Suzuki-Miyaura reaction of aryl halides with phenylboronic acid using a heterogeneous palladium catalyst based on activated carbons(AC) was systematically investigated in this work. Two different reaction modes(batch procedure and continuous-flow procedure) were used to study the variations of reaction processing. The heterogeneous catalysts presented excellent reactivity and recyclability for iodobenzene and bromobenzene substrates in batch mode, which can be attributed to stabilization of Pd nanoparticles by the thiol and amino groups on the AC supports. However, significant dehalogenation in the reaction mixture and Pd leaching from the heterogeneous catalysts were observed in continuous-flow mode.This unique phenomenon in continuous-flow mode resulted in a dramatic decline in reaction selectivity and durability of heterogeneous catalysts comparing with that of batch mode. In addition, the heterogeneous Pd catalysts with thiol-and amino-modified AC supports exhibited different reactivity and durability in batch and continuous-flow mode owing to the difference of interaction between Pd species and AC supports.展开更多
Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-program...Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-programmed reduction （TPR）. Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/（C4 olefin＋C4 paraffin） ratio, and C5 olefin/（C5 olefin＋C5 paraffin） decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.展开更多
The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction（HOR） in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electro...The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction（HOR） in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electrochemical catalytic characteristics of the Pt-Ni/C catalysts.When the Pt mass content was 3.1% percent and that of Ni was 13.9% percent,the Pt-Ni/C-3 catalyst exhibited a larger electrochemically active surface area and a higher exchange current density toward HOR than those of pure supported platinum sample.Our study demonstrates a feasible approach for designing the more efficient catalysts with lower content of noble metal for HOR in fuel cell.展开更多
The dipping method was devised to deposit Pd onto carbon nanotube as supported catalyst(Pd/CNT) for the copolymerization of carbon monoxide(CO) and styrene(ST) towards the formation of polyketone(PK).The Pd/CNT was ch...The dipping method was devised to deposit Pd onto carbon nanotube as supported catalyst(Pd/CNT) for the copolymerization of carbon monoxide(CO) and styrene(ST) towards the formation of polyketone(PK).The Pd/CNT was characterized by X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD) and high-resolution transmission electron microscopy(HRTEM).The construction and crystallization property of PK were evaluated by Fourier transform infrared spectroscopy(FTIR),13C-nuclear magnetic resonance(NMR) and XRD,respectively.The catalyst showed excellent activity and reusability in promoting the fabrication of PK.It can be recycled 14 times with the highest total catalytic activity of 4 239.64 gPK/(gPd·h) at Pd content of 8.63wt%.The results indicate that the prepared catalyst is effective to catalyze the copolymerization of CO and styrene.展开更多
Atmospheric high frequency cold plasma jet was applied to modify Ni/SiO2 catalysts. The catalysts prepared by two different methods with plasma jet were compared with conventional catalysts. BET, XRD, H2-TPD and high-...Atmospheric high frequency cold plasma jet was applied to modify Ni/SiO2 catalysts. The catalysts prepared by two different methods with plasma jet were compared with conventional catalysts. BET, XRD, H2-TPD and high-resolution transmission electron microscopy （HRTEM） were used to characterize these catalysts. The results showed that the catalyst prepared with plasma jet had higher nickel dispersion, larger specific surface area and smaller nickel particle size, about 5 nanometres. Detailed analyses revealed that improved structure and characteristic of the plasma catalyst were benefited from the large amount of hydrogen atoms in the plasma jet, by which the catalyst reduction can be easily achieved in shorter period of time at lower temperature, thus avoiding sintering and conglomeration of the active particles and the support. The activity of catalysts was investigated in the methane reforming with CO2. It is shown that the conversions of CH4 and CO2, the yields of H2 and CO were all significantly increased for the plasma catalysts.展开更多
A series of active carbon supported ruthenium based catalysts, promoted by alkali and alkaline earth nitrate, are prepared by impregnation method and with RuCl 3·3H 2O as precursor. Effects of support, promoter a...A series of active carbon supported ruthenium based catalysts, promoted by alkali and alkaline earth nitrate, are prepared by impregnation method and with RuCl 3·3H 2O as precursor. Effects of support, promoter and preparation conditions on catalytic activity are discussed. The catalytic activity is evaluated with a fixed bed micro reactor at lower pressure. The results show that the impregnation sequence affects the catalytic activity obviously. Ba Ru K/C is the preferred impregnation sequence. And effects of nature, producing area and pre treatment of the support on catalytic activity are also examined. Catalytic activity increases with the amount of Ru deposited on the support, it attains maximum when Ru loading is 8%. Optimal molar ratio of promoter to Ru is 10.展开更多
基金Supported by the Science &Technical Ministry of China( No.2 0 0 1BA3 2 2 C) ,the Science &Technical Department ofFujian Province( No.2 0 0 0 F0 0 2 ) and the Science &Technical Development Foundation of Fuzhou U niversity( No.XKJQD-0 10 2 )
文摘Ten kinds of activated carbon from different raw materials were used as supports to prepare ruthenium catalysts. N_2 physisorption and CO chemisorption were carried out to investigate the pore size distribution and the ruthenium dispersion of the catalysts. It was found that the Ru dispersion of the catalyst was closely related to not only the texture of carbon support but also the purity of activated carbon. The activities of a series of the carbon-supported barium-promoted Ru catalysts for ammonia synthesis were measured at 425 ℃, 10 0 MPa and 10 000 h -1. The result shows that the same raw material activated carbon, with a high purity, high surface area, large pore volume and reasonable pore size distribution might disperse ruthenium and promoter sufficiently, which activated carbon as support, could be used to manufacture ruthenium catalyst with a high activity for ammonia synthesis. The different raw material activated carbon as the support would greatly influence the catalytic properties of the ruthenium catalyst for ammonia synthesis. For example, with coconut shell carbon(AC1) as the support, the ammonia concentration in the effluent was 13 17% over 4%Ru-BaO/AC1 catalyst, while with the desulfurized coal carbon(AC10) as the support, that in the effluent was only 1 37% over 4%Ru-BaO/AC10 catalyst.
基金the support of the National Natural Science Foundation of China (20222809, 21978146)TsinghuaFoshan Innovation Special Fund (2021THFS0214)。
文摘Suzuki-Miyaura reaction of aryl halides with phenylboronic acid using a heterogeneous palladium catalyst based on activated carbons(AC) was systematically investigated in this work. Two different reaction modes(batch procedure and continuous-flow procedure) were used to study the variations of reaction processing. The heterogeneous catalysts presented excellent reactivity and recyclability for iodobenzene and bromobenzene substrates in batch mode, which can be attributed to stabilization of Pd nanoparticles by the thiol and amino groups on the AC supports. However, significant dehalogenation in the reaction mixture and Pd leaching from the heterogeneous catalysts were observed in continuous-flow mode.This unique phenomenon in continuous-flow mode resulted in a dramatic decline in reaction selectivity and durability of heterogeneous catalysts comparing with that of batch mode. In addition, the heterogeneous Pd catalysts with thiol-and amino-modified AC supports exhibited different reactivity and durability in batch and continuous-flow mode owing to the difference of interaction between Pd species and AC supports.
文摘Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-programmed reduction （TPR）. Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/（C4 olefin＋C4 paraffin） ratio, and C5 olefin/（C5 olefin＋C5 paraffin） decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.
基金supported by the National Natural Science Foundation of China (21476145)~~
文摘The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction（HOR） in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electrochemical catalytic characteristics of the Pt-Ni/C catalysts.When the Pt mass content was 3.1% percent and that of Ni was 13.9% percent,the Pt-Ni/C-3 catalyst exhibited a larger electrochemically active surface area and a higher exchange current density toward HOR than those of pure supported platinum sample.Our study demonstrates a feasible approach for designing the more efficient catalysts with lower content of noble metal for HOR in fuel cell.
基金Supported by the National Natural Science Foundation of China(No.20476080)Tianjin Natural Science Foundation(No.07JCYBJC00600)
文摘The dipping method was devised to deposit Pd onto carbon nanotube as supported catalyst(Pd/CNT) for the copolymerization of carbon monoxide(CO) and styrene(ST) towards the formation of polyketone(PK).The Pd/CNT was characterized by X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD) and high-resolution transmission electron microscopy(HRTEM).The construction and crystallization property of PK were evaluated by Fourier transform infrared spectroscopy(FTIR),13C-nuclear magnetic resonance(NMR) and XRD,respectively.The catalyst showed excellent activity and reusability in promoting the fabrication of PK.It can be recycled 14 times with the highest total catalytic activity of 4 239.64 gPK/(gPd·h) at Pd content of 8.63wt%.The results indicate that the prepared catalyst is effective to catalyze the copolymerization of CO and styrene.
基金National Natural Science Foundation of China(No.10475060)the Ministry of Sciences and Technologies of China(2005CB221406)
文摘Atmospheric high frequency cold plasma jet was applied to modify Ni/SiO2 catalysts. The catalysts prepared by two different methods with plasma jet were compared with conventional catalysts. BET, XRD, H2-TPD and high-resolution transmission electron microscopy （HRTEM） were used to characterize these catalysts. The results showed that the catalyst prepared with plasma jet had higher nickel dispersion, larger specific surface area and smaller nickel particle size, about 5 nanometres. Detailed analyses revealed that improved structure and characteristic of the plasma catalyst were benefited from the large amount of hydrogen atoms in the plasma jet, by which the catalyst reduction can be easily achieved in shorter period of time at lower temperature, thus avoiding sintering and conglomeration of the active particles and the support. The activity of catalysts was investigated in the methane reforming with CO2. It is shown that the conversions of CH4 and CO2, the yields of H2 and CO were all significantly increased for the plasma catalysts.
文摘A series of active carbon supported ruthenium based catalysts, promoted by alkali and alkaline earth nitrate, are prepared by impregnation method and with RuCl 3·3H 2O as precursor. Effects of support, promoter and preparation conditions on catalytic activity are discussed. The catalytic activity is evaluated with a fixed bed micro reactor at lower pressure. The results show that the impregnation sequence affects the catalytic activity obviously. Ba Ru K/C is the preferred impregnation sequence. And effects of nature, producing area and pre treatment of the support on catalytic activity are also examined. Catalytic activity increases with the amount of Ru deposited on the support, it attains maximum when Ru loading is 8%. Optimal molar ratio of promoter to Ru is 10.
