Abstract
Surface engineering of bimetallic nanoparticles are crucial for harnessing the true catalytic potential. Herein, H2-induced segregation of palladium was employed to tune the surface structure of PdCo/Al2O3 catalysts with different Pd/Co atomic ratios. The composition dependency of segregation was demonstrated by XRD, XPS, and HAADF-STEM characterization. The results from in situ CO-FTIR analysis show that Pd ensemble sites were formed on Pd75Co25/Al2O3; while, isolated Pd sites were formed on Pd15Co85/Al2O3 after 700 °C hydrogen post-treatment. The post-treated catalysts exhibited significantly increased activity for acetylene selective hydrogenation due to Pd segregation on the surface. In addition, the Pd15Co85-700 catalyst displayed 88% ethene selectivity at ∼100% conversion of acetylene, which was related to the redispersion of Pd and Co during the H2 treatment. Kinetic analysis provided valuable insight into the nature of the active sites resulting from the surface segregation. The Pd15Co85-700 catalyst also showed favorable stability during 100 h reaction.
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