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Unravelling an oxygen-mediated reductive quenching pathway for photopolymerisation under long wavelengths

Nature communications, 2021-01, Vol.12 (1), p.478-478, Article 478 [Peer Reviewed Journal]

The Author(s) 2021. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License. ;The Author(s) 2021 ;ISSN: 2041-1723 ;EISSN: 2041-1723 ;DOI: 10.1038/s41467-020-20640-z ;PMID: 33473121

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  • Title:
    Unravelling an oxygen-mediated reductive quenching pathway for photopolymerisation under long wavelengths
  • Author: Wu, Chenyu ; Jung, Kenward ; Ma, Yongtao ; Liu, Wenjian ; Boyer, Cyrille
  • Subjects: Absorption spectra ; Addition polymerization ; Chain transfer ; Chains (polymeric) ; Deactivation ; Density functional theory ; Electron transfer ; Fragmentation ; Oxygen ; Photocatalysis ; Photocatalysts ; Photopolymerization ; Polymerization ; Porphyrins ; Quenching ; Wavelengths
  • Is Part Of: Nature communications, 2021-01, Vol.12 (1), p.478-478, Article 478
  • Description: Photomediated-reversible-deactivation radical polymerisation (photo-RDRP) has a limited scope of available photocatalysts (PCs) due to multiple stringent requirements for PC properties, limiting options for performing efficient polymerisations under long wavelengths. Here we report an oxygen-mediated reductive quenching pathway (O-RQP) for photoinduced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerisation. The highly efficient polymerisations that are performed in the presence of ambient air enable an expanded scope of available PCs covering a much-broadened absorption spectrum, where the oxygen tolerance of PET-RAFT allows high-quality polymerisation by preventing the existence of O in large amounts and efficient O-RQP is permitted due to its requirement for only catalytic amounts of O . Initially, four different porphyrin dyes are investigated for their ability to catalyse PET-RAFT polymerisation via an oxidative quenching pathway (OQP), reductive quenching pathway (RQP) and O-RQP. Thermodynamic studies with the aid of (time-dependent) density functional theory calculations in combination with experimental studies, enable the identification of the thermodynamic constraints within the OQP, RQP and O-RQP frameworks. This knowledge enables the identification of four phthalocyanine photocatalysts, that were previously thought to be inert for PET-RAFT, to be successfully used for photopolymerisations via O-RQP. Well-controlled polymerisations displaying excellent livingness are performed at wavelengths in the red to near-infrared regions. The existence of this third pathway O-RQP provides an attractive pathway to further expand the scope of photocatalysts compatible with the PET-RAFT process and facile access to photopolymerisations under long wavelengths.
  • Publisher: England: Nature Publishing Group
  • Language: English
  • Identifier: ISSN: 2041-1723
    EISSN: 2041-1723
    DOI: 10.1038/s41467-020-20640-z
    PMID: 33473121
  • Source: PubMed Central
    Directory of Open Access Journals
    ProQuest Central
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