Interplay Between Metal and Acid Sites Tunes the Catalytic Selectivity Over Pd/Nanodiamond Catalysts.

Abstract

Metal and acid sites are two of the most crucial catalytically active components in heterogeneous catalysis. While variations in the size, morphology, and heterogeneity of metal species, or the manipulation of the strength, location, and density of acid sites, could significantly impact the catalytic performance, the combination and interplay between these sites are even more critical and have been a recent research focus. To achieve highly efficient and selective synergistic catalysis, it is desired to design a catalyst capable of orchestrating the sequential transformation of all reactants and intermediates at different active sites. In this study, we demonstrate that both acid and metal (Pd) sites can be introduced onto a nanodiamond@graphene (NDG) support particle through simple air oxidation and metal salt deposition-precipitation methods, respectively. The presence and assembly of these two catalytically active sites significantly alter the reaction network for the cyclohexanol conversion reaction. Under this strategy, the selectivity toward designated products─cyclohexene, phenol, and benzene─can be precisely tuned by the presence and patterning of these two sites on the nanodiamond particles. Specifically, we show that the catalyst with both acid sites and Pd ensemble sites, i.e., Pd/NDG, can efficiently convert cyclohexanol through consecutive dehydration and dehydrogenation reactions to form benzene with high selectivity (>80%). These findings underscore the potential of integrating metal and acid sites to design advanced catalysts with tailored reactivity and selectivity, paving the way for more efficient and versatile catalytic processes in industrial applications.