Enhancing preferential oxidation of CO in H 2 on Au/α-Fe 2O 3 catalyst via combination with APTES/SBA-15 CO 2-sorbent

Abstract

Au/α-Fe 2O 3 was combined with a CO 2-sorbent (3-aminopropyltriethoxysilane (APTES) grafted on SBA-15 and hereafter denoted as APTES/SBA-15) to enhance preferential oxidation (PROX) of CO in H 2. The CO 2 molecules could be rapidly adsorbed on APTES/SBA-15 at low temperatures below 50 °C with a capacity of 0.68 mmol CO 2/g-sample, and desorbed at a temperature range of 50 °C–80 °C. Three different configurations of the Au/α-Fe 2O 3 catalyst and the CO 2-sorbent were tested in the PROX reaction, namely (i) the sorbent-free (catalyst//SBA-15//catalyst) configuration, (ii) the packed three-layer configuration (catalyst//CO 2-sorbent//catalyst), and (iii) the mechanically mixed catalyst and CO 2-sorbent configuration. Compared to configuration (i), configuration (ii) achieved an average 10% higher CO conversion at 50 °C and a GHSV of 65000 h −1. However, the CO concentration could not be lowered to below 70 ppm from 2000 ppm using configuration (ii) at a GHSV of 10000 h −1. Thus, a 5-layer configuration (catalyst//CO 2-sorbent//catalyst//CO 2-sorbent//catalyst) was used, and the CO concentration was lowered to ca. 25 ppm. The mechanism for enhancement of the PROX reaction by the continuous removal of CO 2 by the CO 2-sorbent is discussed and attributed to reduction of the surface carbonate on the Au/α-Fe 2O 3 catalyst formed during the PROX process.