Synthesis of ABC Miktoarm Star Copolymers via Organocatalyzed Living Radical Polymerization

Ge, Yicen; Chen, Chen; Sim, Xuan Ming; Zheng, Jie; Goto, Atsushi

doi:10.1002/marc.201900623

Cited by 8 publications

(3 citation statements)

References 56 publications

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“…RCMP is attractive because of no use of special capping agents or metal catalysts, ease of setup, applicability to a broad scope of monomers (e.g., methacrylates, acrylates, styrene, acrylonitrile, and even steric crowded itaconates), [32][33][34][35][36] and a diversity of polymer designs (e.g., linear, block, star, and brush). [37][38][39][40][41] RCMP has presented versatility due to its high initiator efficiency, narrow polydispersity index (Ð) and moderate reaction rate at high monomer-to-initiator ratios ([M] 0 )/[I] 0 ). This work aims to utilize RCMP to access HMWPs and find their versatile applications (self-assembly) (Scheme 2).…”

Section: Scheme 1 Reversible Activation Of Reversible Complexation-me...mentioning

confidence: 99%

Synthesis of High Molecular Weight Polymers by Organocatalyzed Living Radical Polymerization and Self‐Assembly Behavior

Liu

Zhao

et al. 2023

Macromol. Rapid Commun.

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A mild organocatalyzed living radical polymerization method is studied for high molecular weight polymers (HMWPs), yielding low‐dispersity linear and star polymers (Đ = Mw/Mn = 1.03–1.28) up to Mn = 3.9 × 105 and monomer conversion = 80%, where Mn and Mw are the number‐ and weight‐average molecular weights, respectively. Even at high degrees of polymerization (DPs > 2000), this technique still features excellent control over molecular weights and Đ values, indicating the living character. The macroinitiators prepared at DP = 2000 are subsequently used for block polymerizations at high DPs (>2000) with functional methacrylates, yielding linear A‐B diblock, linear B‐A‐B triblock, and 3‐arm star A‐B diblock copolymers, suggesting the excellent block efficiency of macroinitiators synthesized at a high DP value (=2000). This mild organocatalyzed living radical polymerization technique can enhance the livingness of propagation radicals and kinetic chain length at high monomer conversions for monomers with moderate propagation rate coefficients (kps), reduce the persistent radical effect as much as possible, and hence enable HMWPs without the presence of metal catalyst, exogenous initiator, or harsh equipment. The obtained amphiphilic block copolymers present unique microphase separation behavior, and hold great potential in advanced materials applications, for example, thermosensitive nanocarriers.

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Section: Scheme 1 Reversible Activation Of Reversible Complexation-me...mentioning

confidence: 99%

Synthesis of High Molecular Weight Polymers by Organocatalyzed Living Radical Polymerization and Self‐Assembly Behavior

Liu

Zhao

et al. 2023

Macromol. Rapid Commun.

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“…In 2020, Goto et al synthesized ABC-type miktoarm star copolymers employing RCMP. 46 Their approach uses a single CRP technique (RCMP) and is classified as a “combinatorial” approach. Different from the “core-first” and “coupling-onto” approaches, the “combinatorial” approach does not require the pre-synthesis of special multi-initiating or multi-coupling core molecules that are meticulously designed to avoid the interference of each initiation or coupling reaction.…”

Section: Applicationsmentioning

confidence: 99%

Reversible complexation mediated polymerization: an emerging type of organocatalytically controlled radical polymerization

2022

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“…[ 16–22 ] These synthetic articulations will also continue to strengthen designing miktoarm star‐polymer based formulations with a desired combination of properties for efficient therapeutic interventions. [ 16,22–28 ]…”

Section: Introductionmentioning

confidence: 99%

Miktoarm Star Polymers with Environment‐Selective ROS/GSH Responsive Locations: From Modular Synthesis to Tuned Drug Release through Micellar Partial Corona Shedding and/or Core Disassembly

Lotocki

Yazdani

Zhang

et al. 2020

Macromolecular Bioscience

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Branched architectures with asymmetric polymeric arms provide an advantageous platform for the construction of tailored nanocarriers for therapeutic interventions. Simple and adaptable synthetic methodologies to amphiphilic miktoarm star polymers have been developed in which spatial location of reactive oxygen species (ROS) and glutathione (GSH) responsive entities is articulated to be on the corona shell surface or inside the core. The design of such architectures is facilitated through versatile building blocks and selected combinations of ring‐opening polymerization, Steglich esterification, and alkyne‐azide click reactions. Soft nanoparticles from aqueous self‐assembly of these stimuli responsive miktoarm stars have low critical micelle concentrations and high drug loading efficiencies. Partial corona shedding upon response to ROS is accompanied by an increase in drug release, without significant changes to overall micelle morphology. The location of the GSH responsive unit at the core leads to micelle disassembly and complete drug release. Curcumin loaded soft nanoparticles show higher efficiencies in preventing ROS generation in extracellular and cellular environments, and in ROS scavenging in human glioblastoma cells. The ease in synthetic elaboration and an understanding of structure‐property relationships in stimuli responsive nanoparticles offer a facile venue for well‐controlled drug delivery, based on the extra‐ and intracellular concentrations of ROS and GSH.

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Synthesis of ABC Miktoarm Star Copolymers via Organocatalyzed Living Radical Polymerization

Cited by 8 publications

References 56 publications

Synthesis of High Molecular Weight Polymers by Organocatalyzed Living Radical Polymerization and Self‐Assembly Behavior

Synthesis of High Molecular Weight Polymers by Organocatalyzed Living Radical Polymerization and Self‐Assembly Behavior

Reversible complexation mediated polymerization: an emerging type of organocatalytically controlled radical polymerization

Miktoarm Star Polymers with Environment‐Selective ROS/GSH Responsive Locations: From Modular Synthesis to Tuned Drug Release through Micellar Partial Corona Shedding and/or Core Disassembly

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