Zhang, Ying, Lewis, Richard J., Li, Zhichao, He, Xiaohui, Ji, Hongbing and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560
2025.
Direct synthesis of H2O2 by spatially separate hydrogen and oxygen activation sites on tailored Pt–Au catalysts.
Angewandte Chemie International Edition
, e21118.
10.1002/anie.202521118
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Abstract
The direct synthesis of H2O2 is considered an atom-efficient, environmentally friendly, and sustainable alternative to replace the current industrial route of the anthraquinone oxidation process. To date a viable direct replacement for the current industrial method of H2O2 production has yet to emerge, owing to the strong dissociation abilities of traditional Pd-based catalysts for both H2 and O2, which results in the over hydrogenation of H2O2 and limited catalytic activity. To address these concerns, this work outlines a novel non-Pd-based catalyst (Pt1Aun/TiO2), consisting of spatially separated H2 and O2 activation sites, which offers H2O2 selectivity (∼100%) and productivity (128.6 mol·gN.M.−1·h−1), in excess of state-of-the-art formulations. Crucially, via consecutive reactions, this system achieves net H2O2 concentrations approaching 4 wt.%, which is double that generated in the initial stages of the Anthraquinone Oxidation Process. A detailed mechanistic study indicates that Pt single atoms selectively dissociate H2, while Au nanoparticles stabilize non-dissociative *O2− species. The H2O2 formation proceeds through CH2O-mediated hydrogen transfer, generating a hydrogen carrier (*CH2OH) that subsequently reacts with *O2− to produce H2O2.
| Item Type: | Article |
|---|---|
| Date Type: | Published Online |
| Status: | In Press |
| Schools: | Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI) |
| Publisher: | Wiley |
| ISSN: | 1433-7851 |
| Date of First Compliant Deposit: | 24 November 2025 |
| Date of Acceptance: | 7 November 2025 |
| Last Modified: | 24 Nov 2025 11:15 |
| URI: | https://orca.cardiff.ac.uk/id/eprint/182590 |
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