5 years ago

Directing Reaction Pathways through Controlled Reactant Binding at Pd–TiO2 Interfaces

Directing Reaction Pathways through Controlled Reactant Binding at Pd–TiO2 Interfaces
J. Will Medlin, Jing Zhang, Bingwen Wang, Eranda Nikolla
Recent efforts to design selective catalysts for multi-step reactions, such as hydrodeoxygenation (HDO), have emphasized the preparation of active sites at the interface between two materials having different properties. However, achieving precise control over interfacial properties, and thus reaction selectivity, has remained a challenge. Here, we encapsulated Pd nanoparticles (NPs) with TiO2 films of regulated porosity to gain a new level of control over catalyst performance, resulting in essentially 100 % HDO selectivity for two biomass-derived alcohols. This catalyst also showed exceptional reaction specificity in HDO of furfural and m-cresol. In addition to improving HDO activity by maximizing the interfacial contact between the metal and metal oxide sites, encapsulation by the nanoporous oxide film provided a significant selectivity boost by restricting the accessible conformations of aromatics on the surface. Nanoscale morphology control over active sites consisting of Pd and TiO2 specifies binding orientation of reactant molecules to provide unprecedented reaction specificity toward hydrodeoxygenation during catalytic conversion of biomass-derived aromatic alcohols/aldehydes and phenolics.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201703669

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