Fabrication of highly oxidized Pt single-atom catalysts to suppress the deep hydrogenation of unsaturated aldehydes

In this work, we first reported the fabrication of single-atom Pt catalysts with high oxidation state through a mild hydrolysis method using platinum acetylacetonate as the precursor and SBA-15 coated with functional FeOx nanoclusters as support, and evaluate their catalytic performance towards unsaturated aldehydes hydrogenation. Pt-1-FeOx/SBA-15 featuring the high coordination number of Pt-O exhibited markedly high selectivity for hydrogenation of C--O group (> 95 %) when cinnamaldehyde conversion is 100 %, and further hydrogenation of target product could be efficiently inhibited over a prolonged period of time, and the universality of chemoselectivity was also evidenced in other unsaturated aldehydes. The experimental results and theoretical calculations revealed that the synergism of highly electron-deficient Pt single-atoms and FeOx species is responsible for the selectivity control and the inhibition of further hydrogenation. The developed strategy offers a facile approach to the rational design of high-efficient single-atom catalysts for the selective hydrogenation with multiple intermediates.