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Magnetic Janus nanocomposites with iridium(iii) complexes for heterogeneous catalysis of logic controlled RAFT polymerization using multiplexed external switching

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Abstract

Photoinduced electron/energy transfer-reversible addition–fragmentation chain transfer (PET-RAFT) polymerization has emerged as a versatile and highly-efficient method for the polymerization of more activated monomers including N,N-dimethylacrylamide and methyl acrylate, and less activated monomers including N-vinylpyrrolidone and vinyl acetate, whilst imposing composition, sequence and spatiotemporal regulation. Although significant progress has been achieved in terms of ability to regulate PET-RAFT polymerization through the implementation of myriad environmental cues, it is still a great challenge to introduce multiple external switches within a single catalyst to accomplish logic toggling of controlled radical polymerization (CRP). Herein, we report the synthesis and characterization of Fe3O4@aSiO2@PNMIr Janus nanocomposites coupled with immobilized heteroleptic iridium(III) complexes for heterogeneous catalysis of PET-RAFT polymerization. With this catalytic nanoarchitecture, we demonstrate multi-stimuli switching of CRPs using three different external physical manipulations: light “ON”/“OFF”, magnet “OUT”/“IN” and temperature “LOW”/“HIGH”. In addition, these magnetic Janus nanocomposites endowed radical polymerization with various attractive characteristics such as compatibility of myriad monomer formulations including “more activated” and “less activated” monomers, unique oxygen tolerance and ppm-level catalyst dosage. Logic-controlled polymerization with Fe3O4@aSiO2@PNMIr nanocomposites provides a straightforward, robust and user-friendly strategy for realizing multiplexed external switching of polymer propagation using a single nanocatalyst without the involvement of exogenous reagents.

Graphical abstract: Magnetic Janus nanocomposites with iridium(iii) complexes for heterogeneous catalysis of logic controlled RAFT polymerization using multiplexed external switching

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Supplementary files

Article information


Submitted
14 Jan 2020
Accepted
28 Feb 2020
First published
24 Mar 2020

Nanoscale, 2020, Advance Article
Article type
Paper

Magnetic Janus nanocomposites with iridium(III) complexes for heterogeneous catalysis of logic controlled RAFT polymerization using multiplexed external switching

X. Li, S. Ye, Y. C. Zhang, H. P. Zhao, Y. Huang, B. Zhang and T. Cai, Nanoscale, 2020, Advance Article , DOI: 10.1039/D0NR00402B

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