Chemical reactions at the graphitic step-edge: Changes in product distribution of catalytic reactions as a tool to explore the environment within carbon nanoreactors

Maria A. Lebedeva*, Thomas W. Chamberlain, Alice Thomas, Bradley E. Thomas, Craig T. Stoppiello, Evgeniya Volkova, Mikhail Suetin, Andrei N. Khlobystov

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

A series of explorative cross-coupling reactions have been developed to investigate the local nanoscale environment around catalytically active Pd(ii)complexes encapsulated within hollow graphitised nanofibers (GNF). Two new fullerene-containing and fullerene-free Pd(ii)Salen catalysts have been synthesised, and their activity and selectivity towards different substrates has been explored in nanoreactors. The catalysts not only show a significant increase in activity and stability upon heterogenisation at the graphitic step-edges inside the GNF channel, but also exhibit a change in selectivity affected by the confinement which alters the distribution of isomeric products of the reaction. Furthermore, the observed selectivity changes reveal unprecedented details regarding the location and orientation of the catalyst molecules inside the GNF nanoreactor, inaccessible by any spectroscopic or microscopic techniques, thus shedding light on the precise reaction environment inside the molecular catalyst-GNF nanoreactor.

Original languageEnglish (US)
Pages (from-to)11727-11737
Number of pages11
JournalNanoscale
Volume8
Issue number22
DOIs
StatePublished - Jun 14 2016

ASJC Scopus subject areas

  • Materials Science(all)

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