Assemblies of Polyacrylonitrile-Derived Photoactive Polymers as Blue and Green Light Photo-Cocatalysts for Cu-Catalyzed ATRP in Water and Organic Solvents

Sun, Mingkang; Lorandi, Francesca; Yuan, Rui; Dadashi-Silab, Sajjad; Kowalewski, Tomasz; Matyjaszewski, Krzysztof

doi:10.3389/fchem.2021.734076

Title: Assemblies of Polyacrylonitrile-Derived Photoactive Polymers as Blue and Green Light Photo-Cocatalysts for Cu-Catalyzed ATRP in Water and Organic Solvents

Journal Article · 12 August 2021 · Frontiers in Chemistry

DOI: https://doi.org/10.3389/fchem.2021.734076 · OSTI ID:1813067

Sun, Mingkang ^[1]; Lorandi, Francesca ^[1]; Yuan, Rui ^[1]; Dadashi-Silab, Sajjad ^[1]; Kowalewski, Tomasz ^[1]; Matyjaszewski, Krzysztof ^[1]

Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Chemistry

Photoluminescent nanosized quasi-spherical polymeric assemblies prepared by the hydrothermal reaction of polyacrylonitrile (PAN), ht-PLP_PAN, were demonstrated to have the ability to photo-induce atom transfer radical polymerization (ATRP) catalyzed by low, parts per million concentrations of Cu^II complex with tris(2-pyridylmethyl)amine (TPMA). Such photo induced ATRP reactions of acrylate and methacrylate monomers were performed in water or organic solvents, using ht-PLP_PAN as the photo-cocatalyst under blue or green light irradiation. Mechanistic studies indicate that ht-PLP_PAN helps to sustain the polymerization by facilitating the activation of alkyl bromide species by two modes: 1) green or blue light-driven photoreduction of the Cu^II catalyst to the activating Cu^I form, and 2) direct activation of dormant alkyl bromide species which occurs only under blue light. The photoreduction of the Cu^II complex by ht-PLP_PAN was confirmed by linear sweep voltammetry performed under illumination. Analysis of the polymerization kinetics in aqueous media indicated even though Cu^I complexes comprised only 1–1.4% of all Cu species at equilibrium, they exhibited high activation rate constant and activated the alkyl bromide initiators five to six orders of magnitude faster than ht-PLP_PAN.

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Research Organization:: University of Pittsburgh, PA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: FG02-02ER45998

OSTI ID:: 1813067

Journal Information:: Frontiers in Chemistry, Journal Name: Frontiers in Chemistry Vol. 9; ISSN 2296-2646

Publisher:: Frontiers Research FoundationCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ATRP
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carbon dot
luminescence
photocatalyst
polyacrylonitrile
self-assembly

Title: Assemblies of Polyacrylonitrile-Derived Photoactive Polymers as Blue and Green Light Photo-Cocatalysts for Cu-Catalyzed ATRP in Water and Organic Solvents

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