Solubility and functionality of polymeric materials are essential properties determining their role in any application. In that regard, double hydrophilic copolymers (DHC) are typically constructed from two chemically dissimilar but water-soluble building blocks. During the past decades, these materials have been intensely developed and utilised as, e.g., matrices for the design of multifunctional hybrid materials, in drug carriers and gene delivery, as nanoreactors, or as sensors. This is predominantly due to almost unlimited possibilities to precisely tune DHC composition and topology, their solution behavior, e.g., stimuli-response, and potential interactions with small molecules, ions and (nanoparticle) surfaces. In this contribution we want to highlight that this class of polymers has experienced tremendous progress regarding synthesis, architectural variety, and the possibility to combine response to different stimuli within one material. Especially the implementation of DHCs as versatile building blocks in hybrid materials expanded the range of water-based applications during the last two decades, which now includes also photocatalysis, sensing, and 3D inkjet printing of hydrogels, definitely going beyond already well-established utilisation in biomedicine or as templates.

Double hydrophilic copolymers - synthetic approaches, architectural variety, and current application fields.

The rise of photoredox catalysis has extended the landscape of reversible-deactivation radical polymerization. Recently, visible-light-driven photoredox/Cu dual catalyzed atom transfer radical polymerization (photoATRP) has become an emerging trend, providing well-defined polymer under low copper catalyst loading. In this work, we described a dual catalyzed ATRP using CuBr2/tris(2-pyridinylmethyl)amine (TPMA) and donor–acceptor-type organophotoredox catalysts (OPCs) with visible light absorption. The excited state OPC can reduce both dormant polymer chain-end and CuBr2/TPMA, generating propagating radical species and CuBr/TPMA, respectively. This indicates that the mechanism is a hybrid of organophotoredox-mediated and Cu-mediated ATRP. The photoATRP driven by 425 nm light irradiation produced a series of well-defined polymethacrylates under extremely low catalyst loadings (5 or 10 ppm CuBr2 and 1 ppm OPC relative to monomer). The method also showed excellent temporal control over polymerization and oxygen tolerance. 

Hybrid of Organophotoredox- and Cu-Mediated Pathways Enables Atom Transfer Radical Polymerization with Extremely Low Catalyst Loading

Precise tailoring of thermoresponsive characteristics: Revealing ATRP opportunities for controlled poly(ethylene glycol)-based monomers composition in cyclodextrin-containing polymers

P-doping extended the absorption wavelength of carbon dots (CDs) from the UV-Vis to the NIR region. P-CD-catalyzed NIR-ATRP resulted in a well-controlled polymerization process, as well as temporal control and chain fidelity. 

Phosphorus and nitrogen codoped carbon dots (PN-CDs) catalyzed Vis-NIR light induced photoATRP

Visible-light-induced Decarboxylative Radical Polymerization in Two-Molecule Photoredox System

Thermo- and pH-responsive star-like polymers synthesized by photoATRP

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Thermo- and pH-responsive star-like polymers synthesized by photoATRP