Dual-Atom Catalyst with N-Colligated Zn₁Co₁ Species as Dominant Active Sites for Propane Dehydrogenation

Dual-atom catalysts (DACs) with paired active sites can provide unique intrinsic properties for heterogeneous catalysis, but the synergy of the active centers remains to be elucidated. Here, we develop a high-performance DAC with Zn₁Co₁ species anchored on nitrogen-doped carbon (Zn₁Co₁/NC) as the dominant active site for the propane dehydrogenation (PDH) reaction. It exhibits several times higher turnover frequency (TOF) of C₃H₈ conversion and enhanced C₃H₆ selectivity compared to Zn₁/NC or Co₁/NC with only a single-atom site. Various experimental and theoretical studies suggest that the enhanced PDH performance stems from the promoted activation of the C-H bond of C₃H₈ triggered by the electronic interaction between Zn₁ and Co₁ colligated by N species. Moreover, the dynamic sinking of the Zn₁ site and rising of the Co₁ site, together with the steric effect of the dissociated H species at the bridged N during the PDH reaction, provides a feasible channel for C₃H₆ desorption through the more exposed Co₁ site, thereby boosting the selectivity. This work provides a promising strategy for designing robust hetero DACs to simultaneously increase activity and selectivity in the PDH reaction.