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  1. Article ; Online: Thermoresponsive Poly(

    Ulker, Damla / Neal, Thomas J / Crawford, Aileen / Armes, Steven P

    Biomacromolecules

    2023  Volume 24, Issue 9, Page(s) 4285–4302

    Abstract: RAFT solution polymerization is used to polymerize 2-hydroxypropyl methacrylate (HPMA). The resulting PHPMA precursor is then chain-extended ... ...

    Abstract RAFT solution polymerization is used to polymerize 2-hydroxypropyl methacrylate (HPMA). The resulting PHPMA precursor is then chain-extended using
    MeSH term(s) Humans ; Polymerization ; Cold Temperature ; Gels ; Mesenchymal Stem Cells ; Phase Transition ; Poly A ; Polymers
    Chemical Substances Gels ; Poly A (24937-83-5) ; Polymers
    Language English
    Publishing date 2023-08-24
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ISSN 1526-4602
    ISSN (online) 1526-4602
    DOI 10.1021/acs.biomac.3c00635
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Polymerization-induced self-assembly and disassembly during the synthesis of thermoresponsive ABC triblock copolymer nano-objects in aqueous solution.

    Varlas, Spyridon / Neal, Thomas J / Armes, Steven P

    Chemical science

    2022  Volume 13, Issue 24, Page(s) 7295–7303

    Abstract: Polymerization-induced self-assembly (PISA) has been widely utilized as a powerful methodology for the preparation of various self-assembled AB diblock copolymer nano-objects in aqueous media. Moreover, it is well-documented that chain extension of AB ... ...

    Abstract Polymerization-induced self-assembly (PISA) has been widely utilized as a powerful methodology for the preparation of various self-assembled AB diblock copolymer nano-objects in aqueous media. Moreover, it is well-documented that chain extension of AB diblock copolymer vesicles using a range of
    Language English
    Publishing date 2022-06-08
    Publishing country England
    Document type Journal Article
    ZDB-ID 2559110-1
    ISSN 2041-6539 ; 2041-6520
    ISSN (online) 2041-6539
    ISSN 2041-6520
    DOI 10.1039/d2sc01611g
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Reverse Sequence Polymerization-Induced Self-Assembly in Aqueous Media.

    Neal, Thomas J / Penfold, Nicholas J W / Armes, Steven P

    Angewandte Chemie (International ed. in English)

    2022  Volume 61, Issue 33, Page(s) e202207376

    Abstract: We report a new aqueous polymerization-induced self-assembly (PISA) formulation that enables the hydrophobic block to be prepared first when targeting diblock copolymer nano-objects. This counter-intuitive reverse sequence approach uses an ionic ... ...

    Abstract We report a new aqueous polymerization-induced self-assembly (PISA) formulation that enables the hydrophobic block to be prepared first when targeting diblock copolymer nano-objects. This counter-intuitive reverse sequence approach uses an ionic reversible addition-fragmentation chain transfer (RAFT) agent for the RAFT aqueous dispersion polymerization of 2-hydroxypropyl methacrylate (HPMA) to produce charge-stabilized latex particles. Chain extension using a water-soluble methacrylic, acrylic or acrylamide comonomer then produces sterically stabilized diblock copolymer nanoparticles in an aqueous one-pot formulation. In each case, the monomer diffuses into the PHPMA particles, which act as the locus for the polymerization. A remarkable change in morphology occurs as the ≈600 nm latex is converted into much smaller sterically stabilized diblock copolymer nanoparticles, which exhibit thermoresponsive behavior. Such reverse sequence PISA formulations enable the efficient synthesis of new functional diblock copolymer nanoparticles.
    Language English
    Publishing date 2022-07-06
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.202207376
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article: Block copolymer synthesis in ionic liquid

    Maitland, Georgia L / Liu, Mingyu / Neal, Thomas J / Hammerton, James / Han, Yisong / Worrall, Stephen D / Topham, Paul D / Derry, Matthew J

    Chemical science

    2024  Volume 15, Issue 12, Page(s) 4416–4426

    Abstract: We report for the first time a reversible addition-fragmentation chain transfer polymerisation-induced self-assembly (RAFT-PISA) formulation in ionic liquid (IL) that yields worm gels. A series of poly(2-hydroxyethyl methacrylate)- ...

    Abstract We report for the first time a reversible addition-fragmentation chain transfer polymerisation-induced self-assembly (RAFT-PISA) formulation in ionic liquid (IL) that yields worm gels. A series of poly(2-hydroxyethyl methacrylate)-
    Language English
    Publishing date 2024-02-13
    Publishing country England
    Document type Journal Article
    ZDB-ID 2559110-1
    ISSN 2041-6539 ; 2041-6520
    ISSN (online) 2041-6539
    ISSN 2041-6520
    DOI 10.1039/d3sc06717c
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article: Synthesis and Characterization of Charge-Stabilized Poly(4-hydroxybutyl acrylate) Latex by RAFT Aqueous Dispersion Polymerization: A New Precursor for Reverse Sequence Polymerization-Induced Self-Assembly.

    Buksa, Hubert / Neal, Thomas J / Varlas, Spyridon / Hunter, Saul J / Musa, Osama M / Armes, Steven P

    Macromolecules

    2023  Volume 56, Issue 11, Page(s) 4296–4306

    Abstract: The reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of 4-hydroxybutyl acrylate (HBA) is conducted using a water-soluble RAFT agent bearing a carboxylic acid group. This confers charge stabilization when such ... ...

    Abstract The reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of 4-hydroxybutyl acrylate (HBA) is conducted using a water-soluble RAFT agent bearing a carboxylic acid group. This confers charge stabilization when such syntheses are conducted at pH 8, which leads to the formation of polydisperse anionic PHBA latex particles of approximately 200 nm diameter. The weakly hydrophobic nature of the PHBA chains confers stimulus-responsive behavior on such latexes, which are characterized by transmission electron microscopy, dynamic light scattering, aqueous electrophoresis, and
    Language English
    Publishing date 2023-06-02
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3436-8
    ISSN 0024-9297
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.3c00534
    Database MEDical Literature Analysis and Retrieval System OnLINE

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    In stock of ZB MED Cologne/Königswinter

    Zs.B 1675: Show issues Location:
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  6. Article: Tuning the Glass Transition Temperature of a Core-Forming Block during Polymerization-Induced Self-Assembly: Statistical Copolymerization of Lauryl Methacrylate with Methyl Methacrylate Provides Access to Spheres, Worms, and Vesicles

    György, Csilla / Neal, Thomas J. / Smith, Timothy / Growney, David J. / Armes, Steven P.

    Macromolecules. 2022 May 11, v. 55, no. 10

    2022  

    Abstract: A series of poly(lauryl methacrylate)–poly(methyl methacrylate-stat-lauryl methacrylate) (PLMAₓ–P(MMA-stat-LMA)y) diblock copolymer nanoparticles were synthesized via RAFT dispersion copolymerization of 90 mol % methyl methacrylate (MMA) with 10 mol % ... ...

    Abstract A series of poly(lauryl methacrylate)–poly(methyl methacrylate-stat-lauryl methacrylate) (PLMAₓ–P(MMA-stat-LMA)y) diblock copolymer nanoparticles were synthesized via RAFT dispersion copolymerization of 90 mol % methyl methacrylate (MMA) with 10 mol % lauryl methacrylate (LMA) in mineral oil by using a poly(lauryl methacrylate) (PLMA) precursor with a mean degree of polymerization (DP) of either 22 or 41. In situ ¹H NMR studies of the copolymerization kinetics suggested an overall comonomer conversion of 94% within 2.5 h. GPC analysis confirmed a relatively narrow molecular weight distribution (Mw/Mₙ ≤ 1.35) for each diblock copolymer. Recently, we reported an unexpected morphology constraint when targeting PLMA₂₂–PMMAy nano-objects in mineral oil, with the formation of kinetically trapped spheres being attributed to the relatively high glass transition temperature (Tg) of the PMMA block. Herein we demonstrate that this limitation can be overcome by (i) incorporating 10 mol % LMA into the core-forming block and (ii) performing such syntheses at 115 °C. This new strategy produced well-defined spheres, worms, or vesicles when using the same PLMA₂₂ precursor. Introducing the LMA comonomer not only enhances the mobility of the core-forming copolymer chains by increasing their solvent plasticization but also reduces their effective glass transition temperature to well below the reaction temperature. Copolymer morphologies were initially assigned via transmission electron microscopy (TEM) studies and subsequently confirmed via small-angle X-ray scattering analysis. The thermoresponsive behavior of PLMA₂₂–P(0.9MMA-stat-0.1LMA)₁₁₃ worms and PLMA₂₂–P(0.9MMA-stat-0.1LMA)₂₂₈ vesicles was also studied by using dynamic light scattering (DLS) and TEM. The former copolymer underwent a worm-to-sphere transition on heating from 20 to 170 °C while a vesicle-to-worm transition was observed for the latter. Such thermal transitions were irreversible at 0.1% w/w solids but proved to be reversible at 20% w/w solids.
    Keywords composite polymers ; copolymerization ; glass transition temperature ; mineral oil ; molecular weight ; small-angle X-ray scattering ; solvents
    Language English
    Dates of publication 2022-0511
    Size p. 4091-4101.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 1491942-4
    ISSN 1520-5835 ; 0024-9297
    ISSN (online) 1520-5835
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.2c00475
    Database NAL-Catalogue (AGRICOLA)

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  7. Article: Tuning the Glass Transition Temperature of a Core-Forming Block during Polymerization-Induced Self-Assembly: Statistical Copolymerization of Lauryl Methacrylate with Methyl Methacrylate Provides Access to Spheres, Worms, and Vesicles.

    György, Csilla / Neal, Thomas J / Smith, Timothy / Growney, David J / Armes, Steven P

    Macromolecules

    2022  Volume 55, Issue 10, Page(s) 4091–4101

    Abstract: A series of poly(lauryl methacrylate)-poly(methyl methacrylate- ...

    Abstract A series of poly(lauryl methacrylate)-poly(methyl methacrylate-
    Language English
    Publishing date 2022-05-11
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3436-8
    ISSN 0024-9297
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.2c00475
    Database MEDical Literature Analysis and Retrieval System OnLINE

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    In stock of ZB MED Cologne/Königswinter

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  8. Article: Microstructural Dynamics and Rheology of Worm-like Diblock Copolymer Nanoparticle Dispersions under a Simple Shear and a Planar Extensional Flow.

    Calabrese, Vincenzo / György, Csilla / Haward, Simon J / Neal, Thomas J / Armes, Steven P / Shen, Amy Q

    Macromolecules

    2022  Volume 55, Issue 22, Page(s) 10031–10042

    Abstract: We investigate the shear and extensional flow behavior of dispersions composed of two types of worm-like nanoparticles (WLNPs) with comparable cross-sectional diameters, similar persistence lengths but differing contour lengths, and thus differing ... ...

    Abstract We investigate the shear and extensional flow behavior of dispersions composed of two types of worm-like nanoparticles (WLNPs) with comparable cross-sectional diameters, similar persistence lengths but differing contour lengths, and thus differing flexibility. By measuring the flow-induced birefringence (FIB) of WLNP dispersions in two contrasting microfluidic devices, we obtain an experimental quantification of the role of shearing and planar extensional flows at aligning a short and stiff WLNP (S-WLNP) and a relatively long and flexible WLNP (L-WLNP). We show that shear and extensional flows induce the alignment of both types of WLNPs. However, extensional deformations are more effective than shear deformations at triggering the onset of alignment of the WLNP. The difference between shear and extensional deformations for WLNP alignment is explained based on the ratio of extensional and shear viscosity of the solvent fluid (Trouton ratio of the solvent) and a structural parameter related to the WLNP extensibility and flexibility. Under shear flow, these WLNP dispersions display shear-thinning behavior, with an exponential reduction in viscosity with increasing alignment. Under extensional flow, the WLNP alignment leads to extensional thinning, making WLNP ideal additives for industrial and biotechnology formulations exposed to extensional dominated flows (e.g., jetting, spraying, and printing processes).
    Language English
    Publishing date 2022-10-18
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3436-8
    ISSN 0024-9297
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.2c01314
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  9. Article: Adsorption of Aldehyde-Functional Diblock Copolymer Spheres onto Surface-Grafted Polymer Brushes via Dynamic Covalent Chemistry Enables Friction Modification.

    Johnson, Edwin C / Varlas, Spyridon / Norvilaite, Oleta / Neal, Thomas J / Brotherton, Emma E / Sanderson, George / Leggett, Graham J / Armes, Steven P

    Chemistry of materials : a publication of the American Chemical Society

    2023  Volume 35, Issue 15, Page(s) 6109–6122

    Abstract: Dynamic covalent chemistry has been exploited to prepare numerous examples of adaptable polymeric materials that exhibit unique properties. Herein, the chemical adsorption of aldehyde-functional diblock copolymer spherical nanoparticles onto amine- ... ...

    Abstract Dynamic covalent chemistry has been exploited to prepare numerous examples of adaptable polymeric materials that exhibit unique properties. Herein, the chemical adsorption of aldehyde-functional diblock copolymer spherical nanoparticles onto amine-functionalized surface-grafted polymer brushes via dynamic Schiff base chemistry is demonstrated. Initially, a series of
    Language English
    Publishing date 2023-07-19
    Publishing country United States
    Document type Journal Article
    ZDB-ID 1500399-1
    ISSN 1520-5002 ; 0897-4756
    ISSN (online) 1520-5002
    ISSN 0897-4756
    DOI 10.1021/acs.chemmater.3c01227
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  10. Article ; Online: Enhanced Adsorption of Epoxy-Functional Nanoparticles onto Stainless Steel Significantly Reduces Friction in Tribological Studies.

    György, Csilla / Kirkman, Paul M / Neal, Thomas J / Chan, Derek H H / Williams, Megan / Smith, Timothy / Growney, David J / Armes, Steven P

    Angewandte Chemie (International ed. in English)

    2023  Volume 62, Issue 10, Page(s) e202218397

    Abstract: Epoxy-functional sterically-stabilized diblock copolymer nanoparticles (ca. 27 nm) are prepared via RAFT dispersion polymerization in mineral oil. Nanoparticle adsorption onto stainless steel is examined using a quartz crystal microbalance. Incorporating ...

    Abstract Epoxy-functional sterically-stabilized diblock copolymer nanoparticles (ca. 27 nm) are prepared via RAFT dispersion polymerization in mineral oil. Nanoparticle adsorption onto stainless steel is examined using a quartz crystal microbalance. Incorporating epoxy groups within the steric stabilizer chains results in a two-fold increase in the adsorbed amount, Γ, at 20 °C (7.6 mg m
    Language English
    Publishing date 2023-01-31
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.202218397
    Database MEDical Literature Analysis and Retrieval System OnLINE

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