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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 .

frontiers in chemistry

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