High activity and selectivity of single palladium atom for oxygen hydrogenation to H<sub>2</sub>O<sub>2</sub>.

Yu, Shiming; Cheng, Xing; Wang, Yueshuai; Xiao, Bo; Xing, Yiran; Ren, Jun; Lu, Yue; Li, Hongyi et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

Nanosized palladium (Pd)-based catalysts are widely used in the direct hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) synthesis from H<sub>2</sub> and O<sub>2</sub>, while its selectivity and yield remain inferior because of the O-O bond cleavage from both the reactant O<sub>2</sub> and the produced H<sub>2</sub>O<sub>2</sub>, which is assumed to have originated from various O<sub>2</sub> 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<sub>2</sub> is easier to be activated to form *OOH, which is a key intermediate for H<sub>2</sub>O<sub>2</sub> synthesis; in addition, H<sub>2</sub>O<sub>2</sub> degradation is shut down. Here, we show single Pd atom catalyst displays a remarkable H<sub>2</sub>O<sub>2</sub> yield of 115 mol/g<sub>Pd</sub>/h and H<sub>2</sub>O<sub>2</sub> selectivity higher than 99%; while the concentration of H<sub>2</sub>O<sub>2</sub> reaches 1.07 wt.% in a batch.