Preparation and characterisation of cluster-derived, multimetallic nanoparticles and their catalytic activity in industrially important transformations

Abstract

Multimetallic molecular cluster compounds have been synthesised and characterised. They have been used as precursors for the generation, by heating under vacuum, of nanoparticles supported within the pores of mesoporous silica. By following their activation using infrared spectroscopy, it has been revealed how the temperature of thermolysis determines the nature of the active site.

Through spectroscopic investigations of the active sites, the effect of altering the structure and stoichiometry on the surface metal sites has been elucidated. It has been shown how the inclusion of an oxophilic main group element in the precursor both improves the site isolation of the active sites and affects the oxidation states of the other metals present in the catalyst. The inclusion of an oxophile changes the nature of the bonding between the nanoparticle and the surface and presents different metal atoms at the nanoparticle surface, altering its catalytic activity.

The selection of oxophile is crucial to the activity of the catalyst, since it is possible for it to form a key part of the active site, either purely as a coordination site or indeed as part of the redox system. The use of a molecular cluster precursor greatly enhances this synergistic effect, by ensuring the different metal atoms are chemically bound
throughout catalyst preparation, activation and use.

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Identifiers

ORCID for Robert Raja: orcid.org/0000-0002-4161-7053

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