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Synthesis of Site-specific Charged Metallopolymers via Reversible Addition-Fragmentation Chain Transfer (RAFT) Polymerization.

ABSTRACT: Site-specific cobaltocenium-labeled polymers are synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization using cobaltocenium-labeled chain transfer agents. These chain transfer agents show counterion-dependent solubility. Based on the chemical structure of the chain transfer agents, single cobaltocenium moieties are dictated to be in predetermined locations at either the center or terminals of the polymer chains. Polymerization of hydrophobic monomers (methyl methacrylate, methyl acrylate and styrene) and hydrophilic monomers (2-(dimethylamino)ethyl methacrylate and methacrylic acid) is demonstrated to follow a controlled manner based on kinetic studies. Cobaltocenium-labeled polymers with molecular weights greater than 100,000 Da can be prepared by using a difunctional chain transfer agent. Photophysical properties, electrochemical properties, thermal properties and morphology of the cobaltocenium-labeled polymers are also investigated.

SUBMITTER: Sha Y

PROVIDER: S-EPMC7451713 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Synthesis of Site-specific Charged Metallopolymers via Reversible Addition-Fragmentation Chain Transfer (RAFT) Polymerization.

Sha Ye Y Zhu Tianyu T Rahman Anisur A Cha Yujin Y Hwang Jihyeon J Luo Zhenyang Z Tang Chuanbing C

Polymer 20191217

Site-specific cobaltocenium-labeled polymers are synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization using cobaltocenium-labeled chain transfer agents. These chain transfer agents show counterion-dependent solubility. Based on the chemical structure of the chain transfer agents, single cobaltocenium moieties are dictated to be in predetermined locations at either the center or terminals of the polymer chains. Polymerization of hydrophobic monomers (methyl methac ...[more]

PMID: 32863439

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Project description:Polymerization-induced self-assembly (PISA) is a powerful platform technology for the rational and efficient synthesis of a wide range of block copolymer nano-objects (e.g., spheres, worms or vesicles) in various media. In situ small-angle X-ray scattering (SAXS) studies of reversible addition-fragmentation chain transfer (RAFT) dispersion polymerization have previously provided detailed structural information during self-assembly (see M. J. Derry et al., Chem. Sci. 2016 , 7 , 5078 - 5090 ). However, conducting the analogous in situ SAXS studies during RAFT aqueous emulsion polymerizations poses a formidable technical challenge because the inherently heterogeneous nature of such PISA formulations requires efficient stirring to generate sufficiently small monomer droplets. In the present study, the RAFT aqueous emulsion polymerization of 2-methoxyethyl methacrylate (MOEMA) has been explored for the first time. Chain extension of a relatively short non-ionic poly(glycerol monomethacrylate) (PGMA) precursor block leads to the formation of sterically-stabilized PGMA-PMOEMA spheres, worms or vesicles, depending on the precise reaction conditions. Construction of a suitable phase diagram enables each of these three morphologies to be reproducibly targeted at copolymer concentrations ranging from 10 to 30% w/w solids. High MOEMA conversions are achieved within 2 h at 70 °C, which makes this new PISA formulation well-suited for in situ SAXS studies using a new reaction cell. This bespoke cell enables efficient stirring and hence allows in situ monitoring during RAFT emulsion polymerization for the first time. For example, the onset of micellization and subsequent evolution in particle size can be studied when preparing PGMA29-PMOEMA30 spheres at 10% w/w solids. When targeting PGMA29-PMOEMA70 vesicles under the same conditions, both the micellar nucleation event and the subsequent evolution in the diblock copolymer morphology from spheres to worms to vesicles are observed. These new insights significantly enhance our understanding of the PISA mechanism during RAFT aqueous emulsion polymerization.

Dataset Information

Synthesis of Site-specific Charged Metallopolymers via Reversible Addition-Fragmentation Chain Transfer (RAFT) Polymerization.

Publications

Synthesis of Site-specific Charged Metallopolymers via Reversible Addition-Fragmentation Chain Transfer (RAFT) Polymerization.

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