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Selective Methanation of CO over a Ru-y-AI2O3 Catalyst in CO2 H2

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Selective Methanation of CO over a Ru-y-AI2O3 Catalyst in CO2 H2 ( selective-methanation-co-over-ru-y-ai2o3-catalyst-co2-h2 )

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Energies 2019, 12, 469 3 of 15 on the basis of a 1:1 stoichiometry for the number of Ru atoms exposed on the catalyst surface to the number of chemisorbed H atoms at 110 ◦C. Table 1. Characteristic data of the Ru catalyst. Parameter Particle radius, rp Shell thickness, dsh Density of particle, ρp Porosity of particle, εp Tortuosity, τp Average pore diameter, dpore BET surface area Ru particle size Value 1.25 mm 0.35 mm 980 kg·m−3 0.49 2 9.3 nm 215 m2·g−1 6 nm 2.2. Experimental Set-up The experimental set-up consists of a fixed-bed reactor made of steel with an internal diameter of 1.4 cm and a length of 80 cm. The catalyst was positioned in the middle of the tube and diluted with (inactive) quartz sand in a ratio of 1:2 by mass in order to keep the catalyst temperature constant and to prevent hot spots. The reactor was thermostated by an oil heating system, guaranteeing isothermal conditions. Two thermocouples in a guide tube were positioned in the catalyst bed to monitor the temperature. Feed gases relevant to those of a reformate gas containing CO, CO2, H2, and H2O were used. The concentrations of all these reactants were varied by substituting the reactant of interest by N2, typically 40%, to study the kinetics of each gas; thereby, the inlet concentrations of the other reactants and the total pressure were kept. Experiments took place at atmospheric pressure at temperatures of 160–250 ◦C. The gas composition leaving the reactor (CO, CO2, H2, and CH4) was analyzed with a gas analyzer (X-STREAM Enhanced Process Gas Analyzer, Emerson) and by gas chromatography, although higher hydrocarbons were only formed to a very small extent. The flow rates of the feed gases were adjusted by mass flow controllers and for steam addition by a water saturator. The feed gas could be analyzed by using a bypass. During the kinetic experiments, the gas was directed first to the saturator (in case of steam addition) and then to the reactor and gas analyzer. 2.3. Kinetic Measurements The reactor was charged with 2 g of the catalyst diluted with 4 g of quartz sand. The catalyst bed length was 5 cm. Hence, the pressure drop was considered to be negligible. The measurements were carried out at atmospheric pressure using mixtures of CO, CO2, H2, H2O, and N2. First, the influence of each gas on the reaction rates was examined. Both for CO and for CO2 methanation, a kinetic expression based on a Langmuir–Hinshelwood approach turned out to be suitable. The temperature was then varied from 160–190 ◦C for CO and 190–235 ◦C for CO2. Initially, the residence time was small to keep conversion of CO and CO2 low (<10%) and ensure differential conditions for a direct determination of the rates (ri = − dci/dτ ≈ ci,in Xi/τ). The CO content was varied from 0.4–1.4 vol%, CO2 from 0–20%, H2 from 50–90%, and H2O from 0–20%. Integral kinetic measurements were also conducted to prove the kinetic expressions for a wide range of CO conversion up to almost 100%. 3. Results 3.1. CO Methanation Kinetics As already mentioned, the kinetics of CO methanation follow a Langmuir–Hinshelwood approach: −dCCO =r = kCO(T)cCOcH2 (4) dτ CO 􏰢1 + K1 cCO+K2 cH2O􏰣2

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