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Effect of CeO2 on the catalytic performance of Ni/Al2O3 for autothermal reforming of methane

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Journal of Natural Gas Chemistry 2008年第1期17卷 98-102页

作者： Xiulan Cai xinfa dong Weiming Lin Guangdong Pharmaceutical University Guangzhou 510006 Guangdong China South China University of Technology Guangzhou 510640 Guangdong China

The effect of promoter Ce on the catalytic performance of Ni/Al2O3 catalyst for autothermal reforming of methane to hydrogen was investigated. The catalysts were characterized by X-ray diffraction （XRD）, temperature-programmed reduction （TPR）, and X-ray photoelectron spectroscopy （XPS）. The results indicated that the catalytic performance of the catalysts was improved with the addition of Ce. Ni/Ce30Al70Oδ showed the highest CH4 conversion in operation temperatures ranging from 650 ℃ to 850 ℃. At the same time, the decrease in H2/CO ratio with increasing reaction temperature was consistent with the fact that water-gas shift reaction was thermodynamically unfavorable at higher temperatures. The XRD result indicated that adding Ce to Ni/Al2O3 catalyst prevented the formation of NiAl2O4 and facilitated the formation of NiO. The formation of NiO increased the number of active sites, resulting in higher activity. Comparing the TPR profiles of Ni/Ce30Al70Oδ with Ni/Al2O3, it could be clearly observed that with the addition of Ce, the total reduction peak areas in the middle and low temperatures increased. It was most probably that the addition of Ce inhibited the stronger interaction between Ni and Al2O3 to form the phase of NiAl2O4, and favored the formation of the strong interaction between NiO species and CeO2. Therefore, the addition of Ce to the Ni/Al2O3 catalyst increased the active surface that promoted the activity of the catalyst.

关键词： methane autothermal reforming Ni hydrogen CeO2 co-precipitation

Nickel sulfide modified TiO_2 nanotubes with highly efficient photocatalytic H_2 evolution activity

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Journal of Energy Chemistry 2016年第1期25卷 136-140页

作者： Jiasheng Huang Zhisheng Shi xinfa dong School of Chemistry and Chemical Engineering South China University of Technology

TiO2 nanotubes（TNTs） with nickel sulfide（NiS） co-catalyst were prepared by a simple solvothermal method and characterized by X-ray diffraction, transmission electron microscope, N2-physisorption, UV–vis diffuse reflectance spectroscopy and photoluminescence spectroscopy. Loading NiS nano-clusters can significantly enhance the photocatalytic H2 evolution performance of TNTs. The optimum NiS loading content was found to be 8 wt% and the corresponding hydrogen production rate is ca. 7486 μmol/h/g, being about 79 times higher than that of pure TNTs. This enhancement of photocatalytic H2 evolution was attributed to the synergistic effect between NiS and TNTs.

关键词： Photocatalysis Hydrogen production TiO2 nanotubes NiS

Autothermal Reforming of Methane over Ni Catalysts Supported on CuO-ZrO_2-CeO_2-Al_2O_3

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Journal of Natural Gas Chemistry 2006年第2期15卷 122-126页

作者： Xiulan Cai xinfa dong Weiming Lin School of Chemical and Energy Engineering South China University of Technology Guangzhou 510640 China

Ni catalysts supported on various mixed oxides of Al2O3 with rare earth oxide and transitional metal oxides were synthesized. The studies focused on the measurement of the autothermal reforming of methane to hydrogen over Ni catalysts supported on the mixed oxide ZrxCe30-xAl70Oδ （x-=5, 10, 15）. The catalytic performance of Ni/Zr10Ce20Al70Oδ was better than that of other catalysts. XRD results showed that the addition of Zr to Ni/Ce30Al70Oδ prevented the formation of NiAl2O4 and facilitated the dispersion of NiO. Effects of CuO addition to Zr10Ce20Al70Oδ were also investigated. The activity of Ni catalyst supported on CuO-ZrO2-CeO2-Al2O3 was somewhat affected and the Ni/Cu5Zr10Ce20Al65Oδ showed the best catalytic performance with the highest CH4 conversion, yield of H2, selectivity for H2 and H2/CO production ratio in operation temperatures ranging from 650 to 750 ℃.

关键词： methane autothermal reforming hydrogen nickel-based catalyst ceria zirconia promoter

Preparation and oxygen permeation properties of SrFe(Cu)O_(3-δ) dense ceramic membranes

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Journal of Natural Gas Chemistry 2009年第1期18卷 45-49页

作者： Heng Zhang Tingting Wang xinfa dong Weiming Lin School of Chemistry and Chemical Engineering Qufu Normal University Qufu 273165 Shandong China School of Chemical and Energy Engineering South China University of Technology Guangzhou 510640 Guangdong China

Mixed oxygen-ionic and electronic conducting membranes of SrFe（Cu）O3-δ were prepared by solid-state reaction method. The crystal structure, oxygen nonstoichiometry, and phase stability of the materials were studied by TGA and XRD. Oxygen permeation fluxes through these membranes were studied at operating temperature ranging from 750 to 950 ℃. Results showed that doping Cu in SrFeO3-δ compound had a significant effect on the formation of single-phased perovskite structure. For SrFe1-xCu2O3-δ series materials, the oxygen nonstoichiometry and the oxygen permeation flux increased considerably with the increase of Cu-doping content （x = 0.1-0.3）. The sintering property of the membrane decreased significantly when the Cu substitution amount reached 40%. SrFe0.7Cu0.3O3-δ showed high oxygen permeation flux, but SrCuO2 and Sr2Fe2O5 phases formed in the compound after oxygen permeation test induced cracks in the membrane.

关键词： perovskite mixed conductor oxygen permeation phase stability

Removal of CO from reformed fuels by selective methanation over Ni-B-Zr-O_δ catalysts

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Journal of Natural Gas Chemistry 2009年第2期18卷 173-178页

作者： Qihai Liu xinfa dong Yibing Song Weiming Lin School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510640 Guangdong China College of Science Shantou University Shantou 515063 Guangdong China

The Ni-B-Oδ and Ni-B-Zr-Oδ catalysts were prepared by the method of chemical reduction, and the deep removal of CO by selective methanation from the reformed fuels was performed over the as-prepared catalysts. The results showed that zirconium strongly influenced the activity and selectivity of the Ni-B-Zr-Oδ catalysts. Over the Ni-B-Oδ catalyst, the highest CO conversion obtained was only 24.32% under the experi-mental conditions studied. However, over the Ni-B-Zr-Oδ catalysts, the CO methanation conversion was higher than 90% when the temperature was increased to 220℃. Additionally, it was found that the Ni/B mole ratio also affected the performance of the Ni-B-Zr-Oδ catalysts. With the increase of the Ni/B mole ratio from 1.8 to 2.2, the CO methanation activity of the catalyst was improved. But when the Ni/B mole ratio was higher than 2.2, the performance of the catalyst for CO selective methanation decreased instead. Among all the catalysts, the Ni29B13Zr58Oδ catalyst investigated here exhibited the highest catalytic performance for the CO selective methanation, which was capable of reducing the CO outlet concentration to less than 40 ppm from the feed gases stream in the temperature range of 230-250℃, while the CO2 conversion was kept below 8% all along. Characterization of the Ni-B-Oδ and Ni-B-Zr-Oδ catalysts was provided by XRD, SEM, DSC, and XPS.

关键词： selective methanation CO removal Ni-B-Zr-Oδ catalyst reformed fuels

Effect of Transition Metals (Cu, Co and Fe) on the Autothermal Reforming of Methane over Ni/Ce_(0.2)Zr_(0.1)Al_(0.7)O_δ Catalyst

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Journal of Natural Gas Chemistry 2007年第1期16卷 31-36页

作者： xinfa dong Xiulan Cai Yibing Song Weiming Lin School of Chemical and Energy Engineering South China University of Technology Guangzhou 510640 China Chemistry Department Shantou University Shantou 515063 China

The transition metals （Cu, Co, and Fe） were applied to modify Ni/Ce0.2Zr0.1Al0.7Oδ catalyst. The effects of transition metals on the catalytic properties of Ni/Ce0.2Zr0.1Al0.7Oδ autothermal reforming of methane were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. Tests in autothermal reforming of methane to hydrogen showed that the addition of transition metals （Cu and Co） significantly increased the activity of catalyst under the conditions of lower reaction temperature, and Ni/Cu0.05Ce0.2Zr0.1Al0.65Oδ was found to have the highest conversion of CH4 among all catalysts in the operation temperatures ranging from 923 K to 1023 K. TPR, XRD and XPS measurements indicated that the cubic phases of CexZr1-xO2 solid solution were formed in the preparation process of catalysts. Strong interaction was found to exist between NiO and CexZr1-xO2 solid solution. The addition of Cu improved the dispersion of NiO, inhibited the formation of NiAl2O4, and thus significantly promoted the activity of the catalyst Ni/Cu0.05Ce0.2Zr0.1Al0.65Oδ

关键词： methane autothermal reforming hydrogen Ni-supported catalysts copper CexZr1-xO2 solid solution

Selective CO methanation over amorphous Ni-Ru-B/ZrO_2 catalyst for hydrogen-rich gas purification

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Journal of Natural Gas Chemistry 2010年第5期19卷 497-502页

作者： Qihai Liu Zili Liu LieWen Liao xinfa dong School of Chemistry and Chemical Engineering Zhongkai university of agriculture and engineering Guangzhou 510225 Guangdong China Guangzhou university Guangzhou 510006 Guangdong China School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510640 Guangdong China

Amorphous Ni-Ru-B/ZrO2 catalysts were prepared by chemical reduction method. The effects of Ni-Ru-B loading and Ru/Ni mole ratio on the catalytic performance for selective CO methanation from reformed fuel were studied, and the catalysts were characterized by BET, ICP, XRD and TPD. The results showed that Ru strongly affected the catalytic activity and selectivity by increasing the thermal stability of amorphous structure, promoting the dispersion of the catalyst particle, and intensifying the CO adsorption. For the catalysts with Ru/Ni mole ratio under 0.15, the CO methanation conversion and selectivity increased significantly with the increasing Ru/Ni mole ratio. Among all the catalysts investigated, the 30 wt% Ni-Ru-B loading amorphous Ni61Ru9B30/ZrO2 catalyst with 0.15 Ru/Ni mole ratio presented the best catalytic performance, over which higher than 99.9% of CO conversion was obtained in the temperature range of 230℃-250℃, and the CO2 conversion was kept under the level of 0.9%.

关键词： selective methanation CO hydrogen purification amorphous Ni-Ru-B/ZrO2 catalyst

Carbon Nanotubes Supported Pt-Ru-Ni as Methanol Electro-Oxidation Catalyst for Direct Methanol Fuel Cells

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Journal of Natural Gas Chemistry 2007年第2期16卷 162-166页

作者： Fei Ye Shengzhou Chen xinfa dong Weiming Lin School of Chemical and Energy Engineering South China University of Technology Guangzhou 510640 Guangdong China School of Chemistry and Chemical Engineering Guangzhou University Guangzhou 510006 Guangdong China

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.

关键词： carbon nanotubes Pt-Ru-Ni/CNTs methanol electro-oxidation direct methanol fuel cells

Selective catalytic methanation of CO in hydrogen-rich gases over Ni/ZrO_2 catalyst

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Journal of Natural Gas Chemistry 2008年第3期17卷 268-272页

作者： Qihai Liu xinfa dong Xinman Mo Weiming Lin School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510640 Guangdong China

Ni/ZrO2 catalysts were prepared by the incipient-wetness impregnation method and were investigated in activity and selectivity for the selective catalytic methanation of CO in hydrogen-rich gases with more than 20 vol% CO2. The result showed that Ni loadings significantly influenced the performance of Ni/ZrO2 catalyst. The 1.6 wt% Ni loading catalyst exhibited the highest catalytic activity among all the catalysts in the selective methanation of CO in hydrogen-rich gas. The outlet concentration of CO was less than 20 ppm with the hydrogen consumption below 7%, at a gas-hourly-space velocity as high as 10000 h-1 and a temperature range of 260 °C to 280 °C. The X-ray diffraction （XRD） and temperature programmed reduction （TPR） measurements showed that NiO was dispersed thoroughly on the surface of ZrO2 support if Ni loading was under 1.6 wt%. When Ni loading was increased to 3 wt% or above, the free bulk NiO species began to assemble, which was not favorable to increase the selectivity of the catalyst.

关键词： selective methanation CO removal Ni/ZrO2 catalyst hydrogen-rich gases fuel cell