Revealing the Structure and Mechanism of Palladium during Direct Synthesis of Hydrogen Peroxide in Continuous Flow Using Operando Spectroscopy

The direct synthesis of H2O2 is a dream reaction in the field of selective oxidation and green chemical synthesis. However, the unknown active state of the catalyst and the lack of a defined catalytic mechanism preclude the design and optimization of suitable catalysts and reactor setups. Here direc...

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Bibliographic Details
Published in:ACS catalysis 2018-03, Vol.8 (3), p.2546-2557
Main Authors: Selinsek, Manuel, Deschner, Benedikt J, Doronkin, Dmitry E, Sheppard, Thomas L, Grunwaldt, Jan-Dierk, Dittmeyer, Roland
Format: Article
Language:English
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Summary:The direct synthesis of H2O2 is a dream reaction in the field of selective oxidation and green chemical synthesis. However, the unknown active state of the catalyst and the lack of a defined catalytic mechanism preclude the design and optimization of suitable catalysts and reactor setups. Here direct synthesis of H2O2 over Pd–TiO2 in water was investigated in a continuous flow reactor setup utilizing undiluted oxygen and hydrogen to increase aqueous-phase concentrations safely at ambient temperature and a pressure of 10 bar. In this experiment operando X-ray absorption spectroscopy (XAS) and online flow injection analysis for photometric quantification of H2O2 were combined to build catalyst structure–activity relationships in direct H2O2 synthesis. XAS at the Pd K absorption edge was used to observe the oxidation state and local Pd structure together with H2O2 production for three reactant ratio (H2/O2) regimes: hydrogen rich (>2), hydrogen lean (
ISSN:2155-5435
2155-5435
DOI:10.1021/acscatal.7b03514