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Issue 47, 2016

A fundamental analysis of enhanced cross-coupling catalytic activity for palladium clusters on graphene supports

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Abstract

Combining the recyclability of heterogeneous catalysts with the high activity of ligated homogeneous catalysts for the production of complex organic molecules is a cardinal goal of catalyst development. We have investigated the activity of ultra-fine Pd clusters bound to vacancy defective sites in graphene and found that the defective graphene both serves as a support to stabilize the recyclable catalyst, and also functions as a ligand enhancing the catalytic activity. In this paper, we report computational and experimental results that provide insights into the nature of the interfacial interactions between metal nanoparticles and defect sites on the graphene surface. Theoretical investigations reveal that while the vacancy/void sites on the graphene surface strongly bind to the metal clusters providing enhanced stability against leaching, graphene also serves as a reservoir of electron density that effectively reduces the activation energy of specific steps within the catalytic cycle. Furthermore, multiple experimental methods were used to unambiguously demonstrate that these cross-coupling reactions are occurring at the Pd/G catalyst surface.

Graphical abstract: A fundamental analysis of enhanced cross-coupling catalytic activity for palladium clusters on graphene supports

Supplementary files

Article information


Submitted
26 Aug 2016
Accepted
24 Oct 2016
First published
26 Oct 2016

Nanoscale, 2016,8, 19564-19572
Article type
Paper

A fundamental analysis of enhanced cross-coupling catalytic activity for palladium clusters on graphene supports

Y. Yang, C. E. Castano, B. F. Gupton, A. C. Reber and S. N. Khanna, Nanoscale, 2016, 8, 19564 DOI: 10.1039/C6NR06793J

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