Design of Pt-based Pseudo-binary Intermetallic Catalysts for Dry Reforming of Propane using CO2

Abstract

The utilization of CO₂ along with commercial light alkane dehydrogenation processes has attracted much attention due to the high demand for reducing of CO₂ in the atmosphere caused by human activities and the shale gas boom revolution. Compared with the widely studied dry reforming of methane, converting propane to syngas using CO₂ is more beneficial in terms of easy handling, energy saving and CO₂ utilization efficiency. However, the design of an efficient and stable catalyst remains a challenge due to the difficulty of activating the CO₂ and propane simultaneously. Herein, we report a multifunctional catalyst with a pseudo-binary alloy structure, Pt2CoIn3/CeO₂, which exhibits high activity for C–C bond cleavage and efficient CO₂ activation. As a result, it delivers high CO selectivity and strong coke resistance, maintaining stable performance over 100 h of reaction. Detailed X-ray analyses reveal that the intermetallic structure varies with Co content, which in turn tunes both C₃H₆ adsorptivity and CO₂ activation capability. By combining intermediate surface-reaction studies with density functional theory (DFT) calculations, we identify the difference in the energy barriers for C₃H₆ decomposition and C₃H₆ desorption as a key descriptor governing product selectivity. These findings provide a new design concept for multimetallic catalysts that can be extended to a broad range of selective conversion reactions.