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Enlightening the mechanism of copper mediated photoRDRP via high-resolution mass spectrometry

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Frick, Elena, Anastasaki, Athina, Haddleton, David M. and Barner-Kowollik, Christopher (2015) Enlightening the mechanism of copper mediated photoRDRP via high-resolution mass spectrometry. Journal of the American Chemical Society, 137 (21). pp. 6889-6896. doi:10.1021/jacs.5b03048 ISSN 0002-7863.

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Official URL: http://dx.doi.org/10.1021/jacs.5b03048

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Abstract

The initiation mechanism of photochemically mediated Cu-based reversible-deactivation radical polymerization (photoRDRP) was investigated using pulsed-laser polymerization (PLP) and high-resolution mass spectrometry. The variation of the catalyst composition and ESI-MS analysis of the resulting products provided information on how initiator, ligand, copper species, and monomer are interacting upon irradiation with UV light. A discussion of the results allows for a new postulation of the mechanism of photoRDRP and–for the first time–the unambiguous identification of the initiating species and their interactions within the reaction mixture. One pathway for radical generation proceeds via UV light-induced C–Br bond scission of the initiator, giving rise to propagating radicals. The generation of copper(I) species from copper(II) can occur via several pathways, including, among others, via reduction by free amine ligand in its excited as well as from its ground state via the irradiation with UV light. The amine ligand serves as a strong reducing agent and is likely the main participant in the generation of copper(I) species.

Item Type: Journal Article
Divisions: Faculty of Science, Engineering and Medicine > Science > Chemistry
Journal or Publication Title: Journal of the American Chemical Society
Publisher: American Chemical Society
ISSN: 0002-7863
Official Date: 13 May 2015
Dates:
DateEvent
13 May 2015Published
23 March 2015Submitted
Volume: 137
Number: 21
Page Range: pp. 6889-6896
DOI: 10.1021/jacs.5b03048
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Restricted or Subscription Access

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