Tandem site- and size-controlled Pd nanoparticles for the directed hydrogenation of furfural

Abstract

The conversion of biomass to useful chemical products requires precise catalytic properties to achieve the required activity, selectivity and durability. Here we show, through optimized colloidal synthesis, the tandem control of Pd size and site availability for the directed hydrogenation of the bio-derived intermediate, furfural. Adjusting the temperature of colloidal reduction dictates the size of Pd nanoparticles; in some instances ultra small clusters <20 atoms are achieved. Whereas, changing the solvent system, affects the PVA-Pd interaction and relative proportion of available surface sites (corners, edges, planes), allowing us to control the selectivity to the valuable hydrogenation products of furfuryl alcohol and tetrahydrofurfuryl alcohol. We demonstrate, through combined experimental and computational studies, that Pd nanoparticle planes are more prone to deactivation through the formation of Pd carbide, and the resulting reduced efficacy of furfural binding. This approach to nanoparticle optimization is an important strategy for producing long lasting, high performance catalysts for emerging sustainable technologies.

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ORCID for Peter P. Wells: orcid.org/0000-0002-0859-9172

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