Water-soluble polyphosphonate-based bottlebrush copolymers <i>via</i> aqueous ring-opening metathesis polymerization

Resendiz-Lara, Diego A.; Azhdari, Suna; Gojzewski, Hubert; Gröschel, Andre H.; Wurm, Frederik R.

doi:10.1039/d3sc02649c

Cited by 5 publications

(1 citation statement)

References 69 publications

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“…Ring-opening metathesis polymerization (ROMP) stands out as a highly efficient controlled polymerization technique, allowing for the precise structure and complete monomer conversion within minutes, − thereby providing an effective platform for simultaneous arm synthesis and in situ core formation in a one-pot process. However, a significant challenge associated with the arm-first ROMP approach lies in the inevitable occurrence of intramolecular cross-linking (metathesis reaction of cross-linkers at the one chain end) that greatly restricts the formation of high-molecular-weight star polymers with complete arm conversion.…”

Section: Introductionmentioning

confidence: 99%

Rapid and Efficient Synthesis of Star Polymers via Arm-First Monomer Emulsified Aqueous Ring-Opening Metathesis Polymerization (ME-ROMP)

Hou,

Feng,

Zhou

et al. 2024

Macromolecules

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The combination of ring-opening metathesis polymerization (ROMP) and the arm-first strategy is a widely employed "one-pot two-batch" approach for synthesizing star polymers. However, the intramolecular cross-linking during the core formation in a homogeneous system significantly restricts the production of high-molar-mass star polymers with complete conversion of arms. In this study, we present a successful synthesis of star polymers with diverse chemical compositions and high molar mass using a monomer emulsified ROMP (ME-ROMP) approach based on the arm-first strategy. The arm-first ME-ROMP method involves sequentially injecting CH 2 Cl 2 solution containing a G3 catalyst and hydrophobic cross-linker into aqueous solution of norbornene monomers under stirring. Benefiting from the confinement effect provided by ME-ROMP, the intermolecular cross-linking during core formation was greatly enhanced, resulting in well-defined star polymers with varied chemical compositions and up to 95% conversion of arms within minutes. Furthermore, the star polymers containing cationic copolymer arms exhibited low toxicity and demonstrated potential applications in inflammation inhibition.

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Section: Introductionmentioning

confidence: 99%

Rapid and Efficient Synthesis of Star Polymers via Arm-First Monomer Emulsified Aqueous Ring-Opening Metathesis Polymerization (ME-ROMP)

Hou,

Feng,

Zhou

et al. 2024

Macromolecules

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Ring‐opening metathesis polymerization for synthesizing molecular bottlebrushes via the grafting‐through strategy

Hou,

Yin,

Zhou

et al. 2024

Journal of Polymer Science

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Molecular bottlebrush (MBB) has been considered as an important type of unimolecular nanomaterial for widespread applications ranging from energy to biomedicine, due to its typical one‐dimensional molecular conformation with tunable aspect ratio and chemical composition. In the recently decades, the ring‐opening metathesis polymerization (ROMP) combined with the grafting‐through strategy has emerged as a powerful tool for synthesizing MBBs with various architecture, including (multi)block MBBs, core‐shell MBBs, random MBBs and Janus MBBs et al. In this review, the recent advances on the synthesis of MBBs including the rational preparation of NB terminated macromonomers (MMs) and the grafting‐through ROMP are briefly summarized. Moreover, the emerging progress on the grafting‐through ROMP performed in the aqueous media is also highlighted.

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Degradable Polymer Architectures Based on Polyphosphonate, Poly(2-oxazoline), and Poly(2-oxazine)

Gadaga,

Varanaraja,

Lefley

et al. 2024

Macromolecules

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Degradable polymers are vital, as they reduce environmental impact, conserve resources, and offer biocompatibility for medical applications. Polyphosphoesters (PPE) contain ester bonds in the backbone that enable hydrolytic degradation and are compatible with biological systems. Due to this advantage, PPE have been extensively studied, with efforts to also combine it with other polymer classes. In this study, we demonstrate the successful use of poly(2-oxazoline)s (POx) and poly(2-oxazine)s (POz) as macroinitiators for the ring-opening polymerization of 2-ethyl-2-oxo-1,3,2-dioxaphospholane (EtPPn). POx and POz have been gaining emerging attention in both industrial and biological applications due to their unparalleled synthetic versatility. Therefore, by combination of PPE with this polymer class, the degradability of the former and the unique properties of POx and POz can be exploited for numerous applications. We present a library of novel water-soluble block copolymers and polymeric brushes that combine poly(2-ethyl-2-oxo-1,3,2-dioxaphospholane) (PEtPPn), poly(2-ethyl-2-oxazoline) (PEtOx), and poly(2-n-pentanol-2oxazine) (POzOH). The accelerated degradation of the copolymers is assessed by hydrolysis experiments at pH 11.2 and pH 8.8. The study illustrates that the degradation rate of these novel architectures is modifiable and can be adjusted accordingly to suit different applications.

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Water-soluble polyphosphonate-based bottlebrush copolymers via aqueous ring-opening metathesis polymerization

Abstract: Water-soluble and biodegradable polyphosphoester polymer bottlebrush copolymers and amphiphilic assemblies prepared by a combination of anionic ring-opening and metathesis polymerization.

Cited by 5 publications

References 69 publications

Rapid and Efficient Synthesis of Star Polymers via Arm-First Monomer Emulsified Aqueous Ring-Opening Metathesis Polymerization (ME-ROMP)

Rapid and Efficient Synthesis of Star Polymers via Arm-First Monomer Emulsified Aqueous Ring-Opening Metathesis Polymerization (ME-ROMP)

Ring‐opening metathesis polymerization for synthesizing molecular bottlebrushes via the grafting‐through strategy

Degradable Polymer Architectures Based on Polyphosphonate, Poly(2-oxazoline), and Poly(2-oxazine)

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