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 bioderived intermediate furfural. Adjusting the temperature of colloidal reduction dictates the size of Pd nanoparticles; in some instances ultrasmall clusters of <20 atoms are achieved. However, 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 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, resulting in the reduced efficacy of furfural binding. This approach to nanoparticle optimizat...
Highlights
Upgrading biomass to useful products, be they energy or platform intermediates, is a crucially important part of a sustainable chemicals industry
The B series of Pd/TiO2 produces a larger spread of Pd particle size as a function of preparation temperature, with catalyst PdB2 being smaller than the A series equivalent (PdA1)
For the B series prepared at −30 °C, an average particle size of 1.4 nm was produced, which is smaller than has been previously reported for Pd NPs prepared through a PVA/NaBH4 colloidal route
Summary
Upgrading biomass to useful products, be they energy or platform intermediates, is a crucially important part of a sustainable chemicals industry. The hydrolysis of hemicellulose is one example, where one of the major products, xylose, is acid catalyzed to the valuable intermediate furfural.[1,2] Furfural is readily valorized and is an important precursor in the generation of biofuels[3,4] and chemical intermediates.[2] Furfuryl alcohol, used in the manufacture of resins, adhesives, and synthetic fibers,[5] is produced from the selective hydrogenation of furfural. Subsequent hydrogenation of furfuryl alcohol produces tetrahydrofurfuryl alcohol, a “green solvent”, often used in printer inks and agricultural applications.[6] the hydrogenation of furfural results in a complex network of products (Figure 1), where there is a need to control the relative distribution. The challenge is to find a selective catalyst that has control over C C or C O hydrogenation and disfavors alternative pathways: e.g., decarbonylation
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