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Energies 2019, 12, 469 6 of 15 Energies 2019, 12, x FOR PEER REVIEW 6 of 15 the active catalyst surface (Ru) is blocked by adsorbed CO due to strong adsorption of CO compared and H2O [23]. This leads to a low activity for (dissociative) adsorption of CO2. The kinetic parameters to CO2 and H2O [23]. This leads to a low activity for (dissociative) adsorption of CO2. The kinetic of Equation (6) are presented in Table 3. parameters of Equation (6) are presented in Table 3. Table 3. Parameters of the kinetics of CO2 methanation (see Equations (6) and (7)). Table 3. Parameters of the kinetics of CO2 methanation (see Equations (6) and (7)). Parameter Value Parameter Value EA,CO2 E 81 kJ·mol−1 kA0,CO22 −1 4 861 k−1J·mo−l1 −1 k 0,CO2 4 6 −1 −1 −1 2.8 ×10 m ·s ·kg ·mol K0,3 3 8.4 m ·mol −1 K0,3 ΔH3 ∆H3 8.4 m3·mol−1 15 kJ·mol−1 −1 K0,4 K0,4 15 kJ·mol −13 3 −1 2.8 ×10 m ·s ·kg ·mol 1.15 ×10 −m13 ·m3ol 1.15 ×10 m ·mol −1 −1 −1 Δ∆H4 −12−51k25J·mkJ·omlol 4 K 1.1 3m3 ·m−o1l−1 K5 1.1 m ·mol Note that formally the adsorption of CO2 turned out to be surprisingly endothermic (Table 3). It Note that formally the adsorption of CO2 turned out to be surprisingly endothermic (Table 3). should be also emphasized that, although unsurprisingly the constant K4 for CO “adsorption” in case It should be also emphasized that, although unsurprisingly the constant K4 for CO “adsorption” in of CO2 methanation is at 190°C simil◦ar to the respective parameter K1 for CO methanation, 15 m3 case of CO2 methanation is at 190 C similar to the respective parameter K1 for CO methanation, mol−1 c3ompa−r1edto23m3·mol−1,3(see−E1quation(4)andTables2and3),butK1 turnedouttobe 15 m mol compared to 23 m ·mol , (see Equation (4) and Tables 2 and 3), but K1 turned out to be independent of temperature, whereas the rate of CO2 methanation could only be described accurately independent of temperature, whereas the rate of CO2 methanation could only be described accurately in the whole range of the investigated temperature by assuming a strong influence of temperature on in the whole range of the investigated temperature by assuming a strong influence of temperature on K4. Hence, the physical meaning of the constants Ki, although denoted here as adsorption constants, K4. Hence, the physical meaning of the constants Ki, although denoted here as adsorption constants, is highly questionable, but at least they formally describe the reaction rate(s) quite well. is highly questionable, but at least they formally describe the reaction rate(s) quite well. Figure 3 shows the influence of the CO2 concentration on the reaction rate. The degree of CO2 Figure 3 shows the influence of the CO2 concentration on the reaction rate. The degree of CO2 conversion was kept below 10 % to realize differential conditions (rCO2 = − dcCO2/dτ ≈ cCO2,in XCO2/τ). conversion was kept below 10 % to realize differential conditions (rCO2 = − dcCO2/dτ ≈ cCO2,in The volume rate was 16 to 22 l h−1 (STP). T−h1e agreement of the experimental data and the rates XCO2 /τ). The volume rate was 16 to 22 l h (STP). The agreement of the experimental data and the calculated by Equation (6) is satisfactory. The rate of CO2 methanation increases with increasing CO2 rates calculated by Equation (6) is satisfactory. The rate of CO2 methanation increases with increasing concentration to a maximum and then decreases for high CO2 concentrations (> 5 mol·m−3 = 18 vo−l3- CO2 concentration to a maximum and then decreases for high CO2 concentrations (>5 mol·m = %), as shown in Figure 3 by the calculation for 234 °C and h◦igh values of cCO2. The only product found 18 vol-%), as shown in Figure 3 by the calculation for 234 C and high values of cCO2 . The only product for CO2 conversion is methane, which is a first indication of a negligible activity of the catalyst for the found for CO2 conversion is methane, which is a first indication of a negligible activity of the catalyst RWGS, Equation (3), an aspect discussed below in more detail. for the RWGS, Equation (3), an aspect discussed below in more detail. FigFuigreur3e. 3R.aRteatoeforferaecaticotnionofoCf OC2OwiwthitHh 2H(to(tCoHC4H) a)t adtifdfeifrfenretnint itniaitliaClOC2Oconcocnencetrnattriaotnioant adtifdfeifrfenretnt 224 2 temtepmepraetruatruesre(sm(marakrsk)sc)ocmompapraerdedtotoccaalclcuulalatitoionnssbased on Equation (6) ((solliidlilnineess))(5(55vvool%l%HH,2r, ersetsNt , 22 N 2m, m c a t= = 2 2 g g,, p p = = 1 1 b ba ar r) ). . cat If CO is added to the feed gas containing CO2, the CO2 reaction is strongly suppressed. Figure 4a compares the calculated initial reaction rates of CO and CO2 at different CO concentrations for 190 °C and 230 °C. For clarity, the ratio of both rates is also shown (Figure 4b).PDF Image | Selective Methanation of CO over a Ru-y-AI2O3 Catalyst in CO2 H2
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