Oxygen vacancy-regulated atomic dispersed Au on CeFeOx for preferential oxidation of CO in H2-rich stream

Abstract

CO preferential oxidation in H2-rich stream (CO-PROX) is a critical reaction for H2 purification in emerging hydrogen economy including advanced fuel cell technology. Au-based catalysts are viewed as some of the most promising catalysts but achieving high catalytic efficiency and selectivity is still challenging. Defect engineering is deemed as a powerful strategy to improve the intrinsic catalytic activity. Herein, CeFeOx-supported Au catalysts with controllable oxygen vacancy (Ov) concentrations were obtained and applied to CO-PROX. The results of characterizations showed that the Ovs were preferentially generated in conjunction with Au single atoms (SAs) rather than nanoparticles (NPs), which further modulated the surface electronic properties via surplus electrons in Ovs and enhanced the interfical interaction between Ovs and Au SAs. The CO-PROX results indicated that the reduced Au SA catalyst (Au1/CeFeOx-R) with the highest Ov concentration completely converted CO at temperature of 80 °C with relatively low reactivity towards H2 oxidation. The remarkable catalytic activity and selectivity were attributed to the modified electronic properties by Ovs that played a bridging role in electron transfer and accelerated reaction process, as well as the coupling effect of Ovs and Au SAs that enhanced the dissociative adsorption of O2 and the adsorption-oxidation of CO, resulting in a reduced reaction energy barrier and making CO oxidation more favorable than H2 oxidation. This research opens up an alternative strategy to simultaneously stabilize and activate single-atom catalysts.