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 μmolCO gcat–1 s–1 at atmospheric pressure. Theoretical calculations reveal that the dual-atom Pt–Ni pairs could direct the dual electronic transfer paths (dxz and dyz) to the 2π* 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.