Dual-Atom Catalyst with N-Colligated ZnCo 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 ZnCo species anchored on nitrogen-doped carbon (ZnCo/NC) as the dominant active site for the propane dehydrogenation (PDH) reaction. It exhibits several times higher turnover frequency (TOF) of CH conversion and enhanced CH selectivity compared to Zn/NC or Co/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 CH triggered by the electronic interaction between Zn and Co colligated by N species. Moreover, the dynamic sinking of the Zn site and rising of the Co site, together with the steric effect of the dissociated H species at the bridged N during the PDH reaction, provides a feasible channel for CH desorption through the more exposed Co 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.