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Polymers
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Polymers
Article . 2022
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Polymers
Article . 2022
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Phosphine-Functionalized Core-Crosslinked Micelles and Nanogels with an Anionic Poly(styrenesulfonate) Shell: Synthesis, Rhodium(I) Coordination and Aqueous Biphasic Hydrogenation Catalysis

Authors: Hui Wang; Chantal J. Abou-Fayssal; Christophe Fliedel; Eric Manoury; Rinaldo Poli;

Phosphine-Functionalized Core-Crosslinked Micelles and Nanogels with an Anionic Poly(styrenesulfonate) Shell: Synthesis, Rhodium(I) Coordination and Aqueous Biphasic Hydrogenation Catalysis

Abstract

Stable latexes containing unimolecular amphiphilic core-shell star-block polymers with a triphenylphosphine(TPP)-functionalized hydrophobic core and an outer hydrophilic shell based on anionic styrenesulfonate monomers have been synthesized in a convergent three-step strategy by reversible addition-fragmentation chain-transfer (RAFT) polymerization, loaded with [RhCl(COD)]2 and applied to the aqueous biphasic hydrogenation of styrene. When the outer shell contains sodium styrenesulfonate homopolymer blocks, treatment with a toluene solution of [RhCl(COD)]2 led to undesired polymer coagulation. Investigation of the interactions of [RhCl(COD)]2 and [RhCl(COD)(PPh3)] with smaller structural models of the polymer shell functions, namely sodium p-toluenesulfonate, sodium styrenesulfonate and a poly(sodium styrenesulfonate) homopolymer, in a biphasic toluene/water medium points to the presence of equilibrated Rh-sulfonate interactions as the cause of coagulation by interparticle crosslinking. Modification of the hydrophilic shell to a statistical copolymer of sodium styrenesulfonate and poly(ethylene oxide) methyl ether methacrylate (PEOMA) in a 20:80 ratio allowed particle load-ing with generation of core-anchored [RhCl(COD)TPP] complexes. These Rh-loaded latexes efficiently catalyze the aqueous biphasic hydrogenation of neat styrene as a benchmark reaction. The catalytic phase could be recovered and recycled, although the performances in terms of catalyst leaching and activity evolution during recycles are inferior to those of equivalent nanoreactors based on neutral or polycationic outer shells.

International audience

Countries
France, France, Denmark
Keywords

RAFT polymerization, Polymers and Plastics, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Organic chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, Core-crosslinked micelles, QD241-441, [CHIM.POLY]Chemical Sciences/Polymers, Poly(styrenesulfonate), Polymerization-induced self-assembly, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Aqueous biphasic catalysis, Rhodium, Hydrogenation, aqueous biphasic catalysis; rhodium; hydrogenation; core-crosslinked micelles; poly(styrenesulfonate); RAFT polymerization; polymerization-induced self-assembly

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    This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
    Top 10%
    influence
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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
3
Top 10%
Average
Average
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