One-Pot Synthesis of Block Copolymers in Supercritical Carbon Dioxide: A Simple Versatile Route to Nanostructured Microparticles

Jennings, James; Beija, Mariana; Richez, Alexandre P.; Cooper, Samuel; Mignot, Paul E.; Thurecht, Kristofer J.; Jack, Kevin S.; Howdle, Steven M.

doi:10.1021/ja210577h

Cited by 95 publications

(125 citation statements)

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“…Previous attempts to fabricate discrete, high aspect ratio polymeric structures has proved difficult without the exploitation of exotic chemical properties such as conductivity, which may give rise to undesirable side effects in vivo . 5-8 …”

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confidence: 99%

Injectable Polymeric Cytokine-Binding Nanowires Are Effective Tissue-Specific Immunomodulators

et al. 2017

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Injectable nanomaterials that interact with the host immune system without surgical intervention present spatially anchored complements to cell transplantation and could offer improved pharmacokinetics compared to systemic cytokine therapy. Here we demonstrate fabrication of high aspect ratio polycaprolactone nanowires coupled with cytokine-binding antibodies that assemble into porous matrices when injected into the subcutaneous space. These structures are fabricated using a nanotemplating technique that allows for tunability of particle dimensions and utilize a straightforward maleimide conjugation chemistry to allow site-specific coupling to proteins. Nanowires are well tolerated in vivo and incite minimal inflammatory infiltrate. Nanowires conjugated with antibodies were designed to capture and potentiate endogenous interleukin-2 (IL-2), an important leukocyte activating cytokine. Together these nanowire-antibody matrices were capable of localizing endogenous IL-2 in the skin and activated targeted specific natural killer and T cell subsets, demonstrating both tissue- and cell-specific immune activation. These self-assembling nanowire matrices show promise as scaffolds to present engineered, local receptor–ligand interactions for cytokine-mediated disease.

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confidence: 99%

Injectable Polymeric Cytokine-Binding Nanowires Are Effective Tissue-Specific Immunomodulators

et al. 2017

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“…This idea was reinforced by Zhan et al, who synthesised SBAS by RAFT miniemulsion, which also performed comparably to conventional TPEs despite their high Đ (3) and poorly ordered "sea-island" nanostructure. Self-assembly within block copolymer particles synthesised by RAFT scCO2 dispersion was studied by Jennings et al 119 Phase separated structures were observed in a variety of copolymers, despite some relatively low blocking efficiencies (>50%) and high dispersity (Đ = 2). 120 Particles of symmetrical PMMA-b-PBzMA and PMMA-b-PDMAEMA revealed lamellar phase separated morphology, whilst symmetrical PMMA-b-PSt and PMMAb-P4VP showed cylinders and spheres, respectively (Fig.…”

Section: Figure 8: Afm Images Of Films Prepared From Block (A C) Andmentioning

confidence: 99%

Block copolymer synthesis by controlled/living radical polymerisation in heterogeneous systems

et al. 2016

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Nanostructured soft materials open up new opportunities in material design and application, and block copolymer self-assembly is one particularly powerful phenomenon that can be exploited for their synthesis. The advent of controlled/living radical polymerisation (CLRP) has greatly simplified block copolymer synthesis, and versatility towards monomer types and polymer architectures across the different forms of CLRP has vastly expanded the range of functional materials accessible. CLRP-controlled synthesis of block copolymers has been applied in heterogeneous systems, motivated by the numerous process advantages and the position of emulsion polymerisation at the forefront of industrial latex synthesis. In addition to the inherent environmental advantages of heterogeneous routes, the incidence of block copolymer self-assembly within dispersed particles during polymerisation leads to novel nanostructured materials that offer enticing prospects for entirely new applications of block copolymers. Here, we review the range of block copolymers prepared by heterogeneous CLRP techniques, evaluate the methods applied to maximise purity of the products, and summarise the unique nanoscale morphologies resulting from in situ self-assembly, before discussing future opportunities within the field.2

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“…CO 2 has been exploited as a solvent for polymerisations [7,8], as a foaming agent [1,[9][10][11][12][13], for precipitation/separation [14], particle formation [15,16] and encapsulation [17].…”

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confidence: 99%

High-pressure rheological analysis of CO2-induced melting point depression and viscosity reduction of poly(ε-caprolactone)

Curia

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Howdle

2015

Polymer

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(2015) High-pressure rheological analysis of CO2-induced melting point depression and viscosity reduction of poly(ε-caprolactone). Polymer, Access from the University of Nottingham repository: http://eprints.nottingham.ac.uk/45413/1/curia_polymer2015_preprint.pdf Copyright and reuse:The Nottingham ePrints service makes this work by researchers of the University of Nottingham available open access under the following conditions. This article is made available under the Creative Commons Attribution Non-commercial No Derivatives licence and may be reused according to the conditions of the licence. For more details see: http://creativecommons.org/licenses/by-nc-nd/2.5/ A note on versions:The version presented here may differ from the published version or from the version of record. If you wish to cite this item you are advised to consult the publisher's version. Please see the repository url above for details on accessing the published version and note that access may require a subscription. Furthermore, a significant decrease in the viscosity of two PCL grades with different molecular weight (M n~1 0 kDa and 80 kDa) was also detected upon increasing the CO 2 pressure to 300 bar.Experimental viscosity data were fitted to the Carreau model to quantify the extent of the plasticising effects on the zero-shear viscosity and relaxation time under different conditions. Similar analyses were conducted under high-pressure nitrogen, to compare the effects obtained in the presence of a non-plasticising gas.

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One-Pot Synthesis of Block Copolymers in Supercritical Carbon Dioxide: A Simple Versatile Route to Nanostructured Microparticles

Cited by 95 publications

References 59 publications

Injectable Polymeric Cytokine-Binding Nanowires Are Effective Tissue-Specific Immunomodulators

Injectable Polymeric Cytokine-Binding Nanowires Are Effective Tissue-Specific Immunomodulators

Block copolymer synthesis by controlled/living radical polymerisation in heterogeneous systems

High-pressure rheological analysis of CO2-induced melting point depression and viscosity reduction of poly(ε-caprolactone)

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