Directing reaction pathways by catalyst active-site selection using self-assembled monolayers.

Abstract:

:One key route for controlling reaction selectivity in heterogeneous catalysis is to prepare catalysts that exhibit only specific types of sites required for desired product formation. Here we show that alkanethiolate self-assembled monolayers with varying surface densities can be used to tune selectivity to desired hydrogenation and hydrodeoxygenation products during the reaction of furfural on supported palladium catalysts. Vibrational spectroscopic studies demonstrate that the selectivity improvement is achieved by controlling the availability of specific sites for the hydrogenation of furfural on supported palladium catalysts through the selection of an appropriate alkanethiolate. Increasing self-assembled monolayer density by controlling the steric bulk of the organic tail ligand restricts adsorption on terrace sites and dramatically increases selectivity to desired products furfuryl alcohol and methylfuran. This technique of active-site selection simultaneously serves both to enhance selectivity and provide insight into the reaction mechanism.

journal_name

Nat Commun

journal_title

Nature communications

authors

Pang SH,Schoenbaum CA,Schwartz DK,Medlin JW

doi

10.1038/ncomms3448

subject

Has Abstract

pub_date

2013-01-01 00:00:00

pages

2448

issn

2041-1723

pii

ncomms3448

journal_volume

4

pub_type

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