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Dual-Atom Catalyst with N-Colligated Zn<sub>1</sub>Co<sub>1</sub> Species as Dominant Active Sites for Propane Dehydrogenation

Yicong Chai, Shunhua Chen, Yang Chen, Fenfei Wei, Liru Cao, Jian Lin, Lin Li, Xiaoyan Liu, Sen Lin, Xiaodong Wang, Tao Zhang

2023Journal of the American Chemical Society146 citationsDOI

Abstract

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 Zn 1 Co 1 species anchored on nitrogen-doped carbon (Zn 1 Co 1 /NC) as the dominant active site for the propane dehydrogenation (PDH) reaction. It exhibits several times higher turnover frequency (TOF) of C 3 H 8 conversion and enhanced C 3 H 6 selectivity compared to Zn 1 /NC or Co 1 /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 C 3 H 8 triggered by the electronic interaction between Zn 1 and Co 1 colligated by N species. Moreover, the dynamic sinking of the Zn 1 site and rising of the Co 1 site, together with the steric effect of the dissociated H species at the bridged N during the PDH reaction, provides a feasible channel for C 3 H 6 desorption through the more exposed Co 1 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.

Topics & Concepts

ChemistryDehydrogenationSelectivityCatalysisPropaneActive siteSteric effectsDesorptionPhotochemistryInorganic chemistryStereochemistryPhysical chemistryAdsorptionOrganic chemistryCatalysis and Oxidation ReactionsCatalytic Processes in Materials SciencePhase Equilibria and Thermodynamics