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The direct synthesis of hydrogen peroxide over Au and Pd nanoparticles: A DFT study

Agarwal, N; Thomas, L; Nasrallah, A; Sainna, MA; Freakley, SJ; Edwards, JK; Catlow, CRA; ... Willock, DJ; + view all (2020) The direct synthesis of hydrogen peroxide over Au and Pd nanoparticles: A DFT study. Catalysis Today 10.1016/j.cattod.2020.09.001. (In press). Green open access

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Abstract

Catalysts consisting of Au, Pd and their alloys have been shown to be active oxidation catalysts. These materials can use dioxygen or hydrogen peroxide as the oxidant with CO and activated organic molecules using O_{2}(g) while more challenging cases, such as methane to partial oxygenates, relying on H_{2}O_{2}. Although H_{2}O_{2} is a green oxidant, the incorporation of dioxygen greatly reduces overall cost and so there is an incentive to find new ways to reduce the reliance on H_{2}O_{2}. In this study we use DFT calculations to discuss the direct synthesis of H_{2}O_{2} from H_{2}(g) and O_{2}(g) and use this understanding to identify the important surface species derived from dioxygen. We cover the adsorption of oxygen, hydrogen and water to model Au and Pd nanoclusters and the oxidation of the metals, since reduction of any oxides formed will consume H_{2}. We then turn to the production of a surface hydroperoxy species; the first step in the synthesis of H_{2}O_{2}. This can occur via hydrogenation of O_{2}(ads) with H_{2}(ads) or via protonation of O_{2}(ads) by solvent water. Both routes are found to be energetically reasonable, but the latter is likely to be favoured under experimental conditions.

Type: Article
Title: The direct synthesis of hydrogen peroxide over Au and Pd nanoparticles: A DFT study
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.cattod.2020.09.001
Publisher version: https://doi.org/10.1016/j.cattod.2020.09.001
Language: English
Additional information: © 2020 The Authors. Published by Elsevier B.V. under a Creative Commons license (https://creativecommons.org/licenses/by/4.0/).
Keywords: DFT calculations, Nanoparticles, Oxidation, Catalysis, Hydrogenperoxide, Reaction scheme
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10117202
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