Solvent-mediated charge separation drives alternative hydrogenation path of furanics in liquid water View Full Text


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

2019-04-01

AUTHORS

Zheng Zhao, Reda Bababrik, Wenhua Xue, Yaping Li, Nicholas M. Briggs, Dieu-Thy Nguyen, Umi Nguyen, Steven P. Crossley, Sanwu Wang, Bin Wang, Daniel E. Resasco

ABSTRACT

Compared to the vapour phase, liquid-phase heterogeneous catalysis provides additional degrees of freedom for reaction engineering, but the multifaceted solvent effects complicate analysis of the reaction mechanism. Here, using furfural as an example, we reveal the important role of water-mediated protonation in a typical hydrogenation reaction over a supported Pd catalyst. Depending on the solvent, we have observed different reaction orders with respect to the partial pressure of H2, as well as distinct selectivity towards hydrogenation of the conjugated C=O and C=C double bonds. Free energy calculations show that H2O participates directly in the kinetically relevant reaction step and provides an additional channel for hydrogenation of the aldehyde group, in which hydrogen bypasses the direct surface reaction via a hydrogen-bonded water network. This solution-mediated reaction pathway shows the potential role of the solvent for tuning the selectivity of metal-catalysed hydrogenation when charge separation on the metal surface is feasible. In heterogeneous catalysis, solvents—and their interaction with metal supports—have a complex effect on reactivity. This study shows that, in Pd-catalysed furfural hydrogenation, water influences the rate and selectivity by favouring a proton transfer rather than a purely surface-bound mechanism. More... »

PAGES

1-6

Journal

TITLE

Nature Catalysis

ISSUE

N/A

VOLUME

N/A

From Grant

  • Identifiers

    URI

    http://scigraph.springernature.com/pub.10.1038/s41929-019-0257-z

    DOI

    http://dx.doi.org/10.1038/s41929-019-0257-z

    DIMENSIONS

    https://app.dimensions.ai/details/publication/pub.1113158476


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