Issue 11, 2015

Atomic-scale identification of Pd leaching in nanoparticle catalyzed C–C coupling: effects of particle surface disorder

Abstract

C–C coupling reactions are of great importance in the synthesis of numerous organic compounds, where Pd nanoparticle catalyzed systems represent new materials to efficiently drive these reactions. Despite their pervasive utility, the catalytic mechanism of these particle-based reactions remains highly contested. Herein we present evidence of an atom leaching mechanism for Stille coupling under aqueous conditions using peptide-capped Pd nanoparticles. EXAFS analysis revealed Pd coordination changes in the nanoparticle consistent with Pd atom abstraction, where sizing analysis by SAXS confirmed particle size changes associated with a leaching process. It is likely that recently discovered highly disordered surface Pd atoms are the favored catalytic active sites and are leached during oxidative addition, resulting in smaller particles. Probing the mechanism of nanoparticle-driven C–C coupling reactions through structural analyses provides fundamental information concerning these active sites and their reactivity at the atomic-scale, which can be used to improve catalytic performance to meet important sustainability goals.

Graphical abstract: Atomic-scale identification of Pd leaching in nanoparticle catalyzed C–C coupling: effects of particle surface disorder

Supplementary files

Article information

Article type
Edge Article
Submitted
20 Apr 2015
Accepted
23 Jul 2015
First published
23 Jul 2015
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2015,6, 6413-6419

Atomic-scale identification of Pd leaching in nanoparticle catalyzed C–C coupling: effects of particle surface disorder

B. D. Briggs, N. M. Bedford, S. Seifert, H. Koerner, H. Ramezani-Dakhel, H. Heinz, R. R. Naik, A. I. Frenkel and M. R. Knecht, Chem. Sci., 2015, 6, 6413 DOI: 10.1039/C5SC01424G

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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