Control of selectivity in heterogeneous catalysis by tuning nanoparticle properties and reactor residence time

Elad Gross, Jack Hung Chang Liu, F. Dean Toste*, Gabor A. Somorjai

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

191 Scopus citations

Abstract

A combination of the advantages of homogeneous and heterogeneous catalysis could enable the development of sustainable catalysts with novel reactivity and selectivity. Although heterogeneous catalysts are often recycled more easily than their homogeneous counterparts, they can be difficult to apply in traditional organic reactions and modification of their properties towards a desired reactivity is, at best, complex. In contrast, tuning the properties of homogeneous catalysts by, for example, modifying the ligands that coordinate a metal centre is better understood. Here, using olefin cyclopropanation reactions catalysed by dendrimer-encapsulated Au nanoclusters as examples, we demonstrate that changing the dendrimer properties allows the catalytic reactivity to be tuned in a similar fashion to ligand modification in a homogeneous catalyst. Furthermore, we show that these heterogeneous catalysts employed in a fixed-bed flow reactor allow fine control over the residence time of the reactants and thus enables the control over product distribution in a way that is not easily available for homogeneous catalysts.

Original languageAmerican English
Pages (from-to)947-952
Number of pages6
JournalNature Chemistry
Volume4
Issue number11
DOIs
StatePublished - Nov 2012
Externally publishedYes

Bibliographical note

Funding Information:
We acknowledge support from the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geological and Biosciences of the US Department of Energy (DOE) under contract DE-AC02-05CH11231. Nanoparticle TEM imaging was performed by S. Alayoglu at the Molecular Foundry Imaging Facility, Lawrence Berkeley National Laboratory, which is supported by the Office of Science, Office of Basic Energy Sciences of the US DOE under contract DE-AC02-05CH11231.

Fingerprint

Dive into the research topics of 'Control of selectivity in heterogeneous catalysis by tuning nanoparticle properties and reactor residence time'. Together they form a unique fingerprint.

Cite this