Breaking the Linear Scaling Relationship of the Reverse Water-Gas-Shift Reaction via Construction of Dual-Atom Pt-Ni Pairs

Oxide-supported single-atom catalysts hold great potential for reverse water-gas-shift (RWGS) reactions. Nevertheless, it remains challenging to break the linear scaling relationships between the adsorption and desorption capability of catalysts. Herein, we report the design of ZrO2-anchored dual-atom Pt-Ni pairs for the RWGS reaction. The dual-atom material delivers a CO selectivity as high as 99.8% and a space-time yield of 157.2 mu molCO g(cat)(-1) s(-1) at atmospheric pressure. Theoretical calculations reveal that the dual-atom Pt-Ni pairs could direct the dual electronic transfer paths (d(xz) and d(yz)) to the 2p* orbitals of CO2 in the RWGS reaction, which achieve strong hybridization between them to enable efficient activation of CO2. Moreover, the delocalized charge in dual-atom Pt-Ni may lead to a facile desorption of the CO product.