High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2

Nanosized Pd-based catalysts are widely used in the direct hydrogen peroxide (H2O2) synthesis from H-2 and O-2, while the selectivity and yield of H2O2 remain inferior. Here, a remarkable H2O2 yield of 115 mol/g(Pd)/h and H2O2 selectivity higher than 99% are reported using a Pd single-atom catalyst for the direct synthesis of H2O2. Nanosized palladium (Pd)-based catalysts are widely used in the direct hydrogen peroxide (H2O2) 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 H2O2, 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 H2O2 synthesis; in addition, H2O2 degradation is shut down. Here, we show single Pd atom catalyst displays a remarkable H2O2 yield of 115 mol/g(Pd)/h and H2O2 selectivity higher than 99%; while the concentration of H2O2 reaches 1.07 wt.% in a batch.

Automated summary

Nanosized Pd-based catalysts are commonly used in the direct synthesis of hydrogen peroxide but often achieve low selectivity and yield. This study reports the use of a single-atom Pd catalyst to achieve a remarkable H2O2 yield and selectivity.