Fundamental Studies on Catalytic Reforming of Methane with Steam, Carbondioxide, Oxygen and These Mixed Gas:Mainly Alumina Supported Nickel and Ruthenium Catalysts

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For the purpose to explore catalysts with high activity and durability and a new process for the reforming of CH4, various Al2O3 supported metal catalysts and the effect of the composition of reaction gases were studied. The experiments were carried out by using a flow reactor under an atmospheric pressure and at 450°-950°C. The inlet gases were 10%CH4-10-40%H2O-N2, 10%CH4-10% CO2-N2, 10%CH4-5%02-N2, 10%CH4-5-10%H20-2.5-7%O2-N2, 10%CH4-5%CO2-2.5%O2-N2, 10%CH4-5%H2O-5%CO2-N2, etc., the total feed rate was mainly 1000Ncm3/min per 1ml of each catalyst with average diameter, 0.9mm and space velocity was 6.0×104hr-1. The main results were obtained as follows: (1) The order of apparent activity for steam reforming was 10%Ni>0.3%Ru, 0.3%Rn, 10%Co>0.3%Pt> 0.3%Pd>10%Fe.(2) It is desirable to pre-calcine the commercial γAl2O3 at 11.00°C to form αAl2O3 before the impregnation into Ni (NO3) 2 aq., RuCl3-NH3 complex aq. and etc., and then to reduce in flowing H2 from room temperature to 500°C under increasing and then constant temperature.(3) The synthesis gas (CO+H2) was prepared by using the inlet gases of stoichiometric mole ratio of the following apparent reaction equations. CH4+H2O→CO+3H2, CH4+CO2→2CO+2H2, CH4+ (1/2) O2→CO+2H2, CH4+ (1/2) H2O+ (1/2) O2→CO+ (5/2) H2, CH4+ (1/2) CO2+ (1/2) O2→ (3/2) CO+2H2, CH4+ (1/2) H2O+ (1/2) CO2→ (3/2) CO+ (5/2) H2
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