Impact of Ceria Support Morphology on Au Single‐Atom Catalysts for Benzyl Alcohol Selective Oxidation

Author:

Zhou Xinyue12,Mavridis Aristarchos1,Isaacs Mark A.34,Drivas Charalampos12,D'Agostino Carmine15,Parlett Christopher M. A.126ORCID

Affiliation:

1. Department of Chemical Engineering University of Manchester Manchester M13 9PL UK

2. UK Catalysis Hub Rutherford Appleton Laboratory Oxfordshire OX11 0FA UK

3. HarwellXPS, Rutherford Appleton Labs Oxfordshire OX16 0FA UK

4. Department of Chemistry University College London London WC1H 0AJ UK

5. Dipartimento di Ingegneria Civile Chimica Ambientale e dei Materiali (DICAM), Alma Mater Studiorum – Università di Bologna Via Terracini, 28 40131 Bologna Italy

6. University of Manchester at Harwell, Diamond Light Source Oxfordshire OX11 0DE UK

Abstract

AbstractAlcohol oxidations are a key industrial chemical transformation, with aldehydes and ketones finding use in an array of applications. Nobel metals are known for their activity towards this chemoselective transformation, however, sustainable catalyst synthesis requires optimal utilisation of these scarce elements. Here, we report Au catalytic systems based on the deposition of isolated Au sites on different morphologies of ceria in which different surface facets of the support are exposed. Through tailoring the support morphology and from extensive catalyst characterisation, it is shown that the exposed facet is critical for controlling the formation (or not) of isolated Au sites. Both the 110 and 111 facets are capable of this feat, yielding single‐atom sites for rod, octahedron, and polyhedron morphologies. In contrast, the 100 facet is not, resulting in Au nanoparticles on cubic ceria. This dictation over Au species is critical to benzyl alcohol oxidation capacity at mild conditions and in the absence of a soluble base, with only single‐atom catalyst (SAC) systems demonstrating activity. Furthermore, the exposed surface facet also governs the degree of surface oxygen vacancies, which is critical to catalyst activity due to their control over substrate adsorption strength, as revealed through T1/T2 NMR relaxation measurements.

Funder

Engineering and Physical Sciences Research Council

Diamond Light Source

Publisher

Wiley

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