综述了甲烷水蒸气重整制氢、甲烷部分氧化制氢、甲烷自热重整制氢以及化学链重整制氢等天然气制氢技术的进展,对催化剂的主要研究重点在于提升氢气的选择性、热稳定性、化学稳定性以及抗积炭性等性能。近年来,普遍以镍作为催化剂主体并...综述了甲烷水蒸气重整制氢、甲烷部分氧化制氢、甲烷自热重整制氢以及化学链重整制氢等天然气制氢技术的进展,对催化剂的主要研究重点在于提升氢气的选择性、热稳定性、化学稳定性以及抗积炭性等性能。近年来,普遍以镍作为催化剂主体并运用不同的制备方式向其中添加助剂(Co,Rh,Cu等)和载体(ZrO 2,Al 2O 3,Co 6-x Mg x Al 2等)以提升催化剂性能。将反应过程和分离过程集成、使碳捕集更为便利的化学链制氢技术更具发展前景,催化剂和载氧体的选择是该技术的关键,载氧体需具备低价、稳定、抗积炭以及高活性等性质。除催化剂以外,反应器的种类、原料中杂质的含量、反应加热时燃料的选择、产物中的碳捕集以及氢气提纯装置的选择均为天然气制氢领域的研究要点。展开更多
A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 （x=0, 0.5, 1） were prepared. The structures of the catalysts were characterized using XRD, TPR, T...A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 （x=0, 0.5, 1） were prepared. The structures of the catalysts were characterized using XRD, TPR, TEM and BET techniques. The catalytic activities of the catalysts for steam reforming of methane were evaluated in a continuous flow microreactor. The results indicated that both the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts had good catalytic activities at at- mospheric pressure. The 10wt%Ni/SBA-15 catalyst exhibited excellent stability at 800 ℃ for time on stream of 740 h. After the reaction, carbon deposits were not formed on the surface of the catalyst. There existed a regular hexagonal mesoporous structure in the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts. The nickel species and the CexZr1-xO2 component were all confined in the SBA-15 mesopores. The CexZr1-xO2 could promote dispersion of the nickel species in the Ni/CexZr1-xO2/SBA-15 catalysts.展开更多
Auto-thermal reforming of methane, combining partial oxidation and reforming of methane with CO2 or steam, was carried out with Pt/Al2O3, Pt/ZrO2 and Pt/CeO2 catalysts, in a temperature range of 300-900℃. The auto-th...Auto-thermal reforming of methane, combining partial oxidation and reforming of methane with CO2 or steam, was carried out with Pt/Al2O3, Pt/ZrO2 and Pt/CeO2 catalysts, in a temperature range of 300-900℃. The auto-thermal reforming occurs in two simultaneous stages, namely, total combustion of methane and reforming of the unconverted methane with steam and CO2, with the O2 conversion of 100% starting from 450℃. For combination with CO2 reforming, the Pt/CeO2 catalyst showed the lowest initial activity at 800℃, and the highest stability over 40 h on-stream. This catalyst also presented the best performance for the reaction with steam at 800℃. The higher resistance to coke formation of the catalyst supported on ceria is due to the metal-support interactions and the higher mobility of oxygen in the oxide lattice.展开更多
文摘综述了甲烷水蒸气重整制氢、甲烷部分氧化制氢、甲烷自热重整制氢以及化学链重整制氢等天然气制氢技术的进展,对催化剂的主要研究重点在于提升氢气的选择性、热稳定性、化学稳定性以及抗积炭性等性能。近年来,普遍以镍作为催化剂主体并运用不同的制备方式向其中添加助剂(Co,Rh,Cu等)和载体(ZrO 2,Al 2O 3,Co 6-x Mg x Al 2等)以提升催化剂性能。将反应过程和分离过程集成、使碳捕集更为便利的化学链制氢技术更具发展前景,催化剂和载氧体的选择是该技术的关键,载氧体需具备低价、稳定、抗积炭以及高活性等性质。除催化剂以外,反应器的种类、原料中杂质的含量、反应加热时燃料的选择、产物中的碳捕集以及氢气提纯装置的选择均为天然气制氢领域的研究要点。
基金国家自然科学基金项目“Thermochemical redox cycles for high temperature solar energy conversion into fuels and chemicals”(51950410590)河北省自然科学基金“高炉富氧喷吹煤粉燃烧砷析出机理研究”(E2019209516)。
基金Financial funds from the Chinese Natural Science Foundation(Project No.20473009)the Beijing Natural Science Foundation(Project No.8062023)+1 种基金the National Basic Research Program of China(Project No.2005CB221405)the National"863"Project of China(No.2006 AA10Z425)are gratefully acknowledged.
文摘A series of Ni/SBA-15 catalysts with Ni contents ranging from 5wt% to 20wt% as well as 10wt%Ni/10wt%CexZr1-xO2/SBA-15 （x=0, 0.5, 1） were prepared. The structures of the catalysts were characterized using XRD, TPR, TEM and BET techniques. The catalytic activities of the catalysts for steam reforming of methane were evaluated in a continuous flow microreactor. The results indicated that both the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts had good catalytic activities at at- mospheric pressure. The 10wt%Ni/SBA-15 catalyst exhibited excellent stability at 800 ℃ for time on stream of 740 h. After the reaction, carbon deposits were not formed on the surface of the catalyst. There existed a regular hexagonal mesoporous structure in the Ni/SBA-15 and the Ni/CexZr1-xO2/SBA-15 catalysts. The nickel species and the CexZr1-xO2 component were all confined in the SBA-15 mesopores. The CexZr1-xO2 could promote dispersion of the nickel species in the Ni/CexZr1-xO2/SBA-15 catalysts.
文摘Auto-thermal reforming of methane, combining partial oxidation and reforming of methane with CO2 or steam, was carried out with Pt/Al2O3, Pt/ZrO2 and Pt/CeO2 catalysts, in a temperature range of 300-900℃. The auto-thermal reforming occurs in two simultaneous stages, namely, total combustion of methane and reforming of the unconverted methane with steam and CO2, with the O2 conversion of 100% starting from 450℃. For combination with CO2 reforming, the Pt/CeO2 catalyst showed the lowest initial activity at 800℃, and the highest stability over 40 h on-stream. This catalyst also presented the best performance for the reaction with steam at 800℃. The higher resistance to coke formation of the catalyst supported on ceria is due to the metal-support interactions and the higher mobility of oxygen in the oxide lattice.
