The synthesis of oxide supported Pt-group catalysts typically produces metal particles with dimensions of a few nanometers. Recent work has shown that Pt-group species can co-exist as nanoparticles and single atoms, and that careful synthetic approaches can produce exclusively single atoms. Interest in the reactivity of supported isolated Pt-group metal atoms stems from the maximized metal utilization efficiency, unique reactivity or selectivity, connection to organometallic catalysis, and the potential for making well-defined active sites. It has proven challenging to characterize the intrinsic catalytic activity of these dispersed active sites on oxide supports at a level that relates local electronic and geometric structure to function. The difficulty arises from their atomic dispersion, heterogeneity in the local coordination of active sites on most catalysts (i.e. isolated species sit at different sites on the support), dynamic changes in local coordination under reactive environments, and often the low loading of metal that is required to achieve site isolation.<br/> <br/>In this talk I will describe a synthetic approach to produce isolated Pt-group atoms that exhibit uniformity in their bonding environment on an oxide support and show how a combination of microscopy, spectroscopy and theory can be used to describe the local coordination of these species. Then I will describe two different approaches to control the local environment of Pt-group atoms: (1) through varied pre-treatment that tunes the local coordination and oxidation state of the single atom, and (2) through the addition of inorganic and organic functional groups on the oxide support surrounding the Pt-group atoms. Detailed characterization by a combination of spectroscopy and microscopy is used to develop structure-function relationships for these well-defined single atom active sites in the context of CO oxidation, methanol carbonylation and alkene hydroformylation. This work highlights the ability to tune the local environment of single Pt-group atom active sites on oxide supports in analogous ways to the engineering of organometallic catalysts.<br/>

Controlling the local coordination and reactivity of oxide-supported atomically dispersed Pt-group species

2019 Fall National Meeting

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