High activity and selectivity of single palladium atom for oxygen hydrogenation to H(2)O(2)

Nanosized palladium (Pd)-based catalysts are widely used in the direct hydrogen peroxide (H(2)O(2)) synthesis from H(2) and O(2), while its selectivity and yield remain inferior because of the O-O bond cleavage from both the reactant O(2) and the produced H(2)O(2), which is assumed to have originated from various O(2) adsorption configurations on the Pd nanoparticles. Herein, single Pd atom catalyst with high activity and selectivity is reported. Density functional theory calculations certify that the O-O bond breaking is significantly inhibited on the single Pd atom and the O(2) is easier to be activated to form *OOH, which is a key intermediate for H(2)O(2) synthesis; in addition, H(2)O(2) degradation is shut down. Here, we show single Pd atom catalyst displays a remarkable H(2)O(2) yield of 115 mol/g(Pd)/h and H(2)O(2) selectivity higher than 99%; while the concentration of H(2)O(2) reaches 1.07 wt.% in a batch.