화학공학소재연구정보센터
International Journal of Hydrogen Energy, Vol.44, No.20, 9896-9905, 2019
Utilization of CO2 for syngas production by CH4 partial oxidation using a catalytic membrane reactor
In this research, a synthetic flue gas mixture with added methane was used as the feed gas in the process of dry reforming with partial oxidation of methane using a laboratory scale catalytic membrane reactor to produce hydrogen and carbon monoxide that can present the starting point for methanol or ammonia synthesis and Fischer-Tropsch reactions. 0.5% wt% Rh catalyst was deposited on a gamma-alumina support using rhodium (III) chloride precursor and incorporated into a shell and tube membrane reactor to measure the yield of synthesis gas (CO and H-2) and conversion of CH4, O-2 and CO2 respectively. These measurements were used to determine the reaction order and rate of CO2. The conversion of CO2 and CH4 were determined at different gas hourly space velocities. The reaction order was determined to be a first-order with respect to CO2. The rate of reaction for CO2 was found to follow an Arrhenius equation having an activation energy of 49.88 x 10(-1) kJ mol(-1). Experiments were conducted at 2.5, 5 and 8 ml h(-1) g(-1) gas hourly space velocities and it was observed that increasing the hourly gas velocities resulted in a higher CO2 and CH4 conversions while O-2 conversion remained fairly constant. CO2 had a high conversion rate of 96% at 8 ml h(-1) g(-1). The synthesized catalytic membrane was characterized by Scanning Electron Microscopy (SEM) and the Energy Dispersive X-ray Analysis (EDXA) respectively. The micrographs showed the Rh particles deposited on the alumina support. Single gas permeation of CH4, CO2 and H-2 through the alumina support showed that the permeance of H-2 increased as the pressure was increased to 1 x 10(5) Pa. The order of gas permeance was H-2 (2.00 g/mol) > CH4 (16.04 g/mol) > N-2 (28.01 g/mol) > O-2 (32 g/mol) > CO2 (44.00 g/mol) which is indicative of Knudsen flow mechanism. The novelty of the work lies in the combination of exothermic partial oxidation and endothermic CO2 and steam reforming in a single step in the membrane reactor to achieve near thermoneutrality while simultaneously consuming almost all the greenhouse gases in the feed gas stream. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.