Revealing Intermetallic Active Sites of PtNi Nanocatalysts for Reverse Water Gas Shift Reaction

Bimetallic nanoparticles have gained great interest due to their potential applications in catalysis. By combining Lattice Boltzmann Modeling (LBM), Density Functional Theory (DFT) calculations, and kinetic Monte Carlo (KMC) simulation, here we rationalize the superior performance of supported Pt–Ni alloy nanostructures over Pt and Ni alone during the reverse Water Gas Shift (rWGS) reaction, which was observed previously. The LBM simulation including the diffusion and flow of the reacting gas molecules within the supporting nanoporous channels in SBA-15 indicates that the simple combination of contributions from Ni and Pt alone is not enough to result in the observed promotion in rWGS activity and selectivity of the Pt–Ni alloy. Instead, the synergy between Pt and Ni via a unique intermetallic motif is responsible according to the DFT and KMC simulation. Compared to the monometallic counterparts, the intermetallic-introduced ensemble effect at the low-coordinated Pt–Ni hybrid site of Pt–Ni alloy nanocatalysts enables the enhanced activation of CO2 and promoted removal of CO/H2O as gas phase product.