The effect of non-uniform temperature on the sorption-enhanced steam methane reforming in a tubular fixed-bed reactor

Abstract

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/Al2O3 as the reforming catalyst and CaO as the sorbent. The reaction of SMR is enhanced by removing the CO2 through the reaction of CaO + CO2 → CaCO3 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 CO2 sorption. For a small weight hourly space velocity (WHSV) of 0.67 h−1 before the CO2 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 CH4 conversion and the H2 molar fraction are slightly increased with the increase of D. Based on the parameters adopted in this work, the CH4 conversion, the H2 and CO molar fractions at D = 60 mm are 84.6%, 94.4%, and 0.63%, respectively. After CO2 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 CO2 breakthrough, both the reaction times for SMR and CO2 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 CH4 conversion and H2 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 CH4 conversion and H2 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.