摘要
The effect of non-uniform temperature on the sorption-enhanced steam methane reforming (SE-SMR) in a tubular fixed-bed reactor with a constant wall temperature of 600 °C is investigated numerically by an experimentally verified unsteady two-dimensional model. The reactor uses Ni/Al 2 O 3 as the reforming catalyst and CaO as the sorbent. The reaction of SMR is enhanced by removing the CO 2 through the reaction of CaO + CO 2 → CaCO 3 based on the Le Chatelier's principle. A non-uniform temperature distribution instead of a uniform temperature in the reactor appears due to the rapid endothermic reaction of SMR followed by an exothermic reaction of CO 2 sorption. For a small weight hourly space velocity (WHSV) of 0.67 h −1 before the CO 2 breakthrough, both a low and a high temperature regions exist simultaneously in the catalyst/sorbent bed, and their sizes are enlarged and the temperature distribution is more non-uniform for a larger tube diameter (D). Both the CH 4 conversion and the H 2 molar fraction are slightly increased with the increase of D. Based on the parameters adopted in this work, the CH 4 conversion, the H 2 and CO molar fractions at D = 60 mm are 84.6%, 94.4%, and 0.63%, respectively. After CO 2 breakthrough, the reaction of SMR dominates, and the reactor performance is remarkably reduced due to low reactor temperature. For a higher value of WHSV (4.03 h −1 ) before CO 2 breakthrough, both the reaction times for SMR and CO 2 sorption become much shorter. The size of low temperature region becomes larger, and the high temperature region inside the catalyst/sorbent bed doesn't exist for D ≥ 30 mm. The maximum temperature difference inside the catalyst/sorbent bed is greater than 67 °C. Both the CH 4 conversion and H 2 molar fraction are slightly decreased with the increase of D. However, this phenomenon is qualitatively opposite to that for small WHSV of 0.67 h −1 . The CH 4 conversion and H 2 molar fraction at D = 60 mm are 52.6% and 78.7%, respectively, which are much lower than those for WHSV = 0.67 h −1 .