ORCID Profile
0000-0002-0298-554X
Current Organisation
University of Sydney
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Macromolecular and Materials Chemistry | Synthesis of Materials | Nanochemistry and Supramolecular Chemistry | Nanomaterials | Biomaterials
Expanding Knowledge in the Chemical Sciences | Polymeric Materials (e.g. Paints) | Skeletal System and Disorders (incl. Arthritis) |
Publisher: Wiley
Date: 06-05-2016
Publisher: American Chemical Society (ACS)
Date: 16-05-2014
DOI: 10.1021/LA501324R
Abstract: We report a templating approach for the preparation of functional polymer replica particles via surface-initiated polymerization in mesoporous silica templates. Subsequent removal of the template resulted in discrete polymer particles. Furthermore, redox-responsive replica particles could be engineered to disassemble in a reducing environment. Particles, made of poly(methacryloyloxyethyl phosphorylcholine) (PMPC) or poly[oligo(ethylene glycol) methyl ether methacrylate] (POEGMA), exhibited very low association to human cancer cells (below 5%), which renders the reported charge-neutral polymer particles a modular and versatile class of highly functional carriers with potential applications in drug delivery.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC01601J
Abstract: Molecular polymer bottlebrushes offer a comprehensive toolbox for nanomaterials design. Their tuneable and multifunctional architecture has accelerated their use in nano-bio research and nanomedicine applications.
Publisher: American Chemical Society (ACS)
Date: 29-01-2015
DOI: 10.1021/NN505125F
Abstract: Studies of spherical nanoengineered drug delivery systems have suggested that particle size and mechanical properties are key determinants of in vivo behavior however, for more complex structures, detailed analysis of correlations between in vitro characterization and in vivo disposition is lacking. Anisotropic materials in particular bear unknowns in terms of size tolerances for in vivo clearance and the impact of shape and rigidity. Herein, we employed cylindrical polymer brushes (CPBs) to answer questions related to the impact of size, length and rigidity on the in vivo behavior of PEGylated anisotropic structures, in particular their pharmacokinetics and biodistribution. The modular grafting assembly of CPBs allowed for the systematic tailoring of parameters such as aspect ratio or rigidity while keeping the overall chemical composition the same. CPBs with altered length were produced from polyinitiator backbones with different degrees of polymerization. The side chain grafts consisted of a random copolymer of poly[(ethylene glycol) methyl ether methacrylate] (PEGMA) and poly(glycidyl methacrylate) (PGMA), and rendered the CPBs water-soluble. The epoxy groups of PGMA were subsequently reacted with propargylamine to introduce alkyne groups, which in turn were used to attach radiolabels via copper(I)-catalyzed alkyne-azide cycloaddition (CuAAC). Radiolabeling allowed the pharmacokinetics of intravenously injected CPBs to be followed as well as their deposition into major organs post dosing to rats. To alter the rigidity of the CPBs, core-shell-structured CPBs with polycaprolactone (PCL) as a water-insoluble and crystalline core and PEGMA-co-PGMA as the hydrophilic shell were synthesized. This modular buildup of CPBs allowed their shape and rigidity to be altered, which in turn could be used to influence the in vivo circulation behavior of these anisotropic polymer particles. Increasing the aspect ratio or altering the rigidity of the CPBs led to reduced exposure, higher clearance rates, and increased mononuclear phagocytic system (MPS) organ deposition.
Publisher: American Chemical Society (ACS)
Date: 05-02-2015
DOI: 10.1021/BM5017139
Abstract: Metal-phenolic coordination chemistry provides a simple and rapid way to fabricate ultrathin films. Here, we report a facile strategy for the preparation of low-fouling and pH-degradable metal-phenolic network (MPN) capsules using a synthetic polyphenol derivative, poly(ethylene glycol) (PEG)-polyphenol, as a building block. PEG-MPN capsules exhibit reduced nonspecific protein adsorption and cell association compared with tannic acid (TA)-MPN capsules. In addition, they show faster disassembly at a biologically relevant pH (5) than TA-MPN capsules (80% in 5 h vs 30% in 10 days). PEG-MPN capsules combine both the low fouling properties of PEG and the advantages of the MPN-driven assembly process (e.g., fast assembly and pH-degradability).
Publisher: Wiley
Date: 29-07-2020
Publisher: Wiley
Date: 02-05-2018
Abstract: Understanding the self-assembly behavior of polymers of various topologies is key to a reliable design of functional polymer materials. Self-assembly under confinement conditions emerges as a versatile avenue to design polymer particles with complex internal morphologies while simultaneously facilitating scale-up. However, only linear block copolymers have been studied to date, despite the increasing control over macromolecule composition and architecture available. This study extends the investigation of polymer self-assembly in confinement from regular diblock copolymers to diblock molecular polymer brushes (MPBs). Block-type MPBs with polystyrene (PS) and polylactide (PLA) compartments of different sizes are incorporated into surfactant-stabilized oil-in-water (chloroform/water) emulsions. The increasing confinement in the nanoemulsion droplets during solvent evaporation directs the MPBs to form solid nano/microparticles. Microscopy studies reveal an intricate internal particle structure, including interpenetrating networks and axially stacked lamellae of PS and PLA, depending on the PS/PLA ratio of the brushes.
Publisher: American Chemical Society (ACS)
Date: 26-02-2016
DOI: 10.1021/ACS.BIOMAC.6B00027
Abstract: Particles with tailored geometries have received significant attention due to their specific interactions with biological systems. In this work, we examine the effect of polymer capsule shape on cytokine secretion by human monocyte-derived macrophages. Thiolated poly(methacrylic acid) (PMASH) polymer capsules with different shapes (spherical, short rod-shaped, and long rod-shaped) were prepared by layer-by-layer assembly. The effect of PMASH capsule shape on cellular uptake and cytokine secretion by macrophages differentiated from THP-1 monocytes (dTHP-1) was investigated. PMASH capsules with different shapes were internalized to a similar extent in dTHP-1 cells. However, cytokine secretion was influenced by capsule geometry: short rod-shaped PMASH capsules promoted a stronger increase in TNF-α and IL-8 secretion compared with spherical (1.7-fold in TNF-α and 2.1-fold in IL-8) and long rod-shaped (2.8-fold in TNF-α and 2.0-fold in IL-8) PMASH capsules in dTHP-1 cells (capsule-to-cell ratio of 100:1). Our results indicate that the immunological response based on the release of cytokines is influenced by the shape of the polymer capsules, which could be potentially exploited in the rational design of particle carriers for vaccine delivery.
Publisher: American Chemical Society (ACS)
Date: 13-01-2015
DOI: 10.1021/MZ5007443
Publisher: American Chemical Society (ACS)
Date: 04-05-2012
DOI: 10.1021/CM300312G
Publisher: Wiley
Date: 27-02-2022
Abstract: Nanoparticle (NP)‐based drug delivery systems are promising in anticancer therapy, capable of delivering cargo with superior selectivity and achieving enhanced tumor accumulation compared to small‐molecule therapeutics. As more efforts are being devoted to NP development, molecular polymer bottlebrushes (MPBs) have gained attention as a potential drug delivery vehicle. To date, the influence of various MPB parameters such as size, shape, and surface charge in determining tumor penetrability have been systematically probed. However, the role of hiphilicity, specifically the hydrophilic–hydrophobic balance, remains unexplored. In this study, a series of MPBs are employed with varied hydrophobicity levels to reveal a dependence between MPB composition, cell association, and tumor homing. The data indicates that increasing levels of hydrophobicity in MPBs (to a certain level) demonstrate only marginal effects in vitro but reveals enhanced tumor homing in a mouse model of ovarian cancer in vivo, where more hydrophilic MPBs exhibit low tissue deposition and low tumor homing. In contrast, more hydrophobic MPBs show significant tumor accumulation and homing due to their engineered hydrophobicity.
Publisher: American Chemical Society (ACS)
Date: 28-10-2010
DOI: 10.1021/JA107132J
Abstract: We report the preparation of water-soluble organo-silica hybrid nanotubes templated by core-shell-corona structured triblock terpolymer cylindrical polymer brushes (CPBs). The CPBs consist of a polymethacrylate backbone, a poly(tert-butyl acrylate) (PtBA) core, a poly(3-(trimethoxysilyl)propyl acrylate) (PAPTS) shell, and a poly(oligo(ethylene glycol) methacrylate) (POEGMA) corona. They were prepared via the "grafting from" strategy by the combination of two living/controlled polymerization techniques: anionic polymerization for the backbone and atom transfer radical polymerization (ATRP) for the triblock terpolymer side chains. The monomers tBA, APTS, and OEGMA were consecutively grown from the pendant ATRP initiating groups along the backbone to spatially organize the silica precursor, the trimethoxysilyl groups, into a tubular manner. The synthesized core-shell-corona structured CPBs then served as a unimolecular cylindrical template for the in situ fabrication of water-soluble organo-silica hybrid nanotubes via base-catalyzed condensation of the PAPTS shell block. The formed tubular nanostructures were characterized by transmission electron microscopy (TEM), cryogenic TEM, and atomic force microscopy.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8PY00703A
Abstract: Molecular polymer brushes allow for independent tailoring of nanoparticle design parameters. Brush particles with altered shape and aspect ratio revealed that particle shape effects may be decoupled from surface chemistry to achieve higher tumour spheroid interaction and penetration.
Publisher: American Chemical Society (ACS)
Date: 06-08-2015
Publisher: Wiley
Date: 05-2019
Publisher: American Chemical Society (ACS)
Date: 27-09-2018
DOI: 10.1021/JACS.8B08870
Abstract: The construction of precise soft matter nanostructures in solution presents a challenge. A key focus remains on the rational design of functionalities to achieve the high morphological complexity typically found in biological systems. Advances in controlled polymerizations and self-assembly increasingly allow approaches toward complex hierarchical nanomaterials. By combining tailor-made cylindrical polymer brushes, block copolymers and interpolyelectrolyte complexation-driven self-assembly, we demonstrate a facile construction of uniformly compartmentalized and topographically structured polymeric nanowires in aqueous media. The approach offers a modular avenue in programming the internal morphology of polymer nanowires by varying the block copolymer composition and topology.
Publisher: American Chemical Society (ACS)
Date: 10-02-2014
DOI: 10.1021/CM403903M
Publisher: American Chemical Society (ACS)
Date: 26-08-2021
Publisher: Wiley
Date: 10-02-2009
Abstract: The synthesis of several diblock copolymers with DMAEMA via anionic polymerization is presented PS ‐b‐ PDMAEMA, PB ‐b‐ PDMAEMA, poly( p ‐ tert‐ butoxystyrene) ‐b‐ PDMAEMA, and PEO ‐b‐ PDMAEMA. The latter was synthesized using sec ‐butyllithium as initiator in presence of the phosphazene base t ‐BuP 4 , enabling a facile changeover from an oxyanion to a carbanion. All reactions resulted in narrowly distributed block copolymers (PDI 1.1). For PEO ‐b‐ PDMAEMA, diblock copolymers with a high blocking efficiency and a near‐narrow molecular weight distribution (PDI 1.40) could be prepared. The advantage of the presented one‐pot synthesis is a significant higher blocking efficiency compared to commercially available PEO macroinitiators under similar conditions. magnified image
Publisher: Wiley
Date: 29-05-2012
Abstract: High-aspect-ratio rutile and anatase hybrid nanowires are produced via a template-directed process using a novel cylindrical polyelectrolyte brush template. Loading the highly negatively charged 1D templates with pre-synthesized TiO(2) nanocrystals, results in the fabrication of soluble crystalline TiO(2) hybrid nanowires.
Publisher: American Chemical Society (ACS)
Date: 25-07-2013
DOI: 10.1021/LA402146T
Abstract: Soft hydrogel particles with tunable mechanical properties are promising for next-generation therapeutic applications. This is due to the increasingly proven role that physicochemical properties play in particulate-based delivery vectors, both in vitro and in vivo. The ability to understand and quantify the mechanical properties of such systems is therefore essential to optimize function and performance. We report control over the mechanical properties of poly(methacrylic acid) (PMA) hydrogel particles based on a mesoporous silica templating method. The mechanical properties of the obtained particles can be finely tuned through variation of the cross-linker concentration, which is hereby quantified using a cross-linking polymer with a fluorescent tag. We demonstrate that the mechanical properties of the particles can be elucidated using an atomic force microscopy (AFM) force spectroscopy method, which additionally allows for the study of hydrogel material properties at the nanoscale through high-resolution force mapping. Young's modulus and stiffness of the particles were tuned between 0.04 and 2.53 MPa and between 1.6 and 28.4 mN m(-1), respectively, through control over the cross-linker concentration. The relationship between the concentration of the cross-linker added and the amount of adsorbed polymer was observed to follow a Langmuir isotherm, and this relationship was found to correlate linearly with the particle mechanical properties.
Publisher: Elsevier BV
Date: 05-2014
DOI: 10.1016/J.CIS.2013.10.012
Abstract: Hollow polymer capsules are attracting increasing research interest due to their potential application as drug delivery vectors, sensors, biomimetic nano- or multi-compartment reactors and catalysts. Thus, significant effort has been directed toward tuning their size, composition, morphology, and functionality to further their application. In this review, we provide an overview of emerging techniques for the fabrication of polymer capsules, encompassing: self-assembly, layer-by-layer assembly, single-step polymer adsorption, bio-inspired assembly, surface polymerization, and ultrasound assembly. These techniques can be applied to prepare polymer capsules with erse functionality and physicochemical properties, which may fulfill specific requirements in various areas. In addition, we critically evaluate the challenges associated with the application of polymer capsules in drug delivery systems.
Publisher: Elsevier BV
Date: 03-2017
Publisher: American Chemical Society (ACS)
Date: 23-08-2012
DOI: 10.1021/MA301232M
Publisher: Wiley
Date: 07-09-2010
Publisher: American Chemical Society (ACS)
Date: 06-2016
DOI: 10.1021/ACS.BIOMAC.6B00537
Abstract: We engineered metal-phenolic capsules with both high targeting and low nonspecific cell binding properties. The capsules were prepared by coating phenolic-functionalized hyaluronic acid (HA) and poly(ethylene glycol) (PEG) on calcium carbonate templates, followed by cross-linking the phenolic groups with metal ions and removing the templates. The incorporation of HA significantly enhanced binding and association with a CD44 overexpressing (CD44+) cancer cell line, while the incorporation of PEG reduced nonspecific interactions with a CD44 minimal-expressing (CD44-) cell line. Moreover, high specific targeting to CD44+ cells can be balanced with low nonspecific binding to CD44- cells simply by using an optimized feed-ratio of HA and PEG to vary the content of HA and PEG incorporated into the capsules. Loading an anticancer drug (i.e., doxorubicin) into the obtained capsules resulted in significantly higher cytotoxicity to CD44+ cells but lower cytotoxicity to CD44- cells.
Publisher: American Chemical Society (ACS)
Date: 16-11-2019
DOI: 10.1021/ACS.JPCLETT.9B02993
Abstract: The optical and electronic properties of π-conjugated polymers in organic electronic devices depend on their intra- and interchain interactions, dictated by the internal arrangement of the polymer chains in an amorphous or semicrystalline aggregated state. Here, we discuss the utility of circular intensity differential scattering (CIDS) of circularly polarized light as a sensitive probe to identify the internal arrangement of the polymer chains in helical polymer aggregates. We advance existing theoretical models to utilize the CIDS response and extract structural properties such as the size, orientation, and periodicity of a polymer aggregate. As an ex le, we analyze the CIDS signatures of helically assembled fibrillar aggregates of a chiral polymer poly[(9,9-di-
Publisher: Informa UK Limited
Date: 04-08-2020
Publisher: American Chemical Society (ACS)
Date: 15-12-2020
Publisher: American Chemical Society (ACS)
Date: 30-11-2018
DOI: 10.1021/ACS.CHEMRESTOX.8B00120
Abstract: Three-dimensional (3D) hepatocyte microtissues (MT), also known as spheroids, have proven to be advantageous in providing more accurate information and physiologically relevant and predictive data for liver-related in vivo tests therefore, spheroids have increasingly been used to study hepatotoxicity, drug delivery to the liver, and tissue engineering. However, variabilities in the generation of 3D MT remain a major challenge. Methods that encapsulate and protect hepatocytes offer a promising pathway in prolonging cell survival, as well as maintaining its liver cell functions. Herein, we studied the encapsulation and resultant protective effects of hydrogen bonded, biocompatible polymer coatings for hepatocyte MT in 3D cell culture. We exposed the MT to hepatotoxic nanomaterials (NMs), such as graphene oxide (GO) and cobalt oxide (Co
Publisher: Wiley
Date: 09-01-2019
Publisher: American Chemical Society (ACS)
Date: 23-02-2023
Publisher: Wiley
Date: 14-05-2018
Publisher: American Chemical Society (ACS)
Date: 06-2020
Publisher: Cold Spring Harbor Laboratory
Date: 02-06-2022
DOI: 10.1101/2022.06.02.494465
Abstract: The utility of CRISPR in plants has remained limited by the dual difficulties of delivering the molecular machinery to target cells and the use of somatic cell techniques that require tissue culture-based de novo organogenesis. We developed 5-10 nm isodiametric polyplex nanoassemblies, comprising poly [2-(dimethylamino)ethylmethacrylate] PDMAEMA (PD) polycationic linear homopolymers and CRISPR/Cas9 ribonucleoproteins (RNPs), that enable endocytosis-driven RNP uptake into pollen grains. Pollen from wheat plants (genotype Gladius+Sr50), homozygous for monogenic Sr50 -mediated resistance to stem rust ( Puccinia graminis f. sp. tritici -Pgt), were incubated with RNP/PD nanoassemblies targeting the dominant, Sr50 rust resistance gene. The treated pollen grains were then used to fertilize Gladius+Sr50 florets and the resulting M1 plants were tested for loss of Sr50 function via rust resistance screens. The identification of fully susceptible M1 seedlings indicated that the Sr50 RNPs acted on both alleles, indicating they were transferred via the treated pollen to the zygote. The ability to readily deliver CRISPR RNPs to reproductive cells via biodegradable, polymeric nanocomplexes has significant implications for the efficiency of gene editing in plants.
Publisher: Elsevier BV
Date: 08-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3PY00194F
Abstract: Polymer brush-grafted cellulose nanocrystals can be used as rod-like nanoreactors to produce carbon-coated titania nanocomposites for battery anodes.
Publisher: MDPI AG
Date: 28-07-2023
DOI: 10.3390/GELS9080611
Abstract: Chronic wounds, depending on the bacteria that caused the infection, can be associated with an extreme acidic or basic pH. Therefore, the application of pH-responsive hydrogels has been instigated for the delivery of therapeutics to chronic wounds. Herein, with the aim of developing a flexible pH-responsive hydrogel, we functionalized hydrophilic polyurethanes with either cationic (polyethylene imine) or anionic (succinic anhydride) moieties. A comprehensive physicochemical characterization of corresponding polymers was carried out. Particularly, when tested in aqueous buffers, the surface charge of hydrogel films was closely correlated with the pH of the buffers. The loading of the cationic and anionic hydrogel films with various compound models (bromophenol blue negatively charged or Pyronin Y positively charged) showed that the electrostatic forces between the polymeric backbone and the compound model will determine the ultimate release rate at any given pH. The potential application of these films for chronic wound drug delivery was assessed by loading them with an antibiotic (ciprofloxacin). In vitro bacterial culturing was performed using Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). Results showed that at the same drug dosage, different release profiles achievable from cationic and anionic polyurethanes can yield different degrees of an antibacterial effect. Overall, our results suggest the potential application of cationic and anionic hydrophilic polyurethanes as flexible pH-responsive materials for the delivery of therapeutics to chronic wounds.
Publisher: American Chemical Society (ACS)
Date: 11-11-2013
DOI: 10.1021/MA401799G
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6NR02151D
Abstract: Understanding the behaviour of therapeutic carriers is important in elucidating their mechanism of action and how they are processed inside cells. Herein we examine the intracellular deformation of layer-by-layer assembled polymer capsules using super-resolution structured illumination microscopy (SIM). Spherical- and cylindrical-shaped capsules were studied in three different cell lines, namely HeLa (human epithelial cell line), RAW264.7 (mouse macrophage cell line) and differentiated THP-1 (human monocyte-derived macrophage cell line). We observed that the deformation of capsules was dependent on cell line, but independent of capsule shape. This suggests that the mechanical forces, which induce capsule deformation during cell uptake, vary between cell lines, indicating that the capsules are exposed to higher mechanical forces in HeLa cells, followed by RAW264.7 and then differentiated THP-1 cells. Our study demonstrates the use of super-resolution SIM in analysing intracellular capsule deformation, offering important insights into the cellular processing of drug carriers in cells and providing fundamental knowledge of intracellular mechanobiology. Furthermore, this study may aid in the design of novel drug carriers that are sensitive to deformation for enhanced drug release properties.
Publisher: American Chemical Society (ACS)
Date: 20-09-2019
Publisher: Wiley
Date: 23-12-2018
DOI: 10.1002/POLA.29312
Publisher: American Chemical Society (ACS)
Date: 21-12-2009
DOI: 10.1021/BM901099P
Abstract: We report a general and facile approach for the fabrication of a new class of near monodisperse hybrid nanoparticles via RAFT polymerization and self-assembly in water. Furthermore, we combine a fluorescent inorganic silica core with a biocompatible polymer shell and a terminal unit susceptible to facile conjugations via click chemistry. A tailoring of the weight fractions of both components allows a tuning of the size of the formed aggregates. Fluorescent properties and the crosslinking into an organic-inorganic hybrid network are realized by copolymerizing a dye-functionalized monomer 1-pyrenebutyl acrylate and a trimethoxysilane-carrying one, (3-acryloxypropyl)trimethoxysilane. The potential of these stabilized and fluorescent nanoparticles as biocompatible carriers for intracellular delivery is demonstrated via in vitro experiments on lung cancer cells.
Publisher: Wiley
Date: 20-02-2013
Publisher: Elsevier BV
Date: 08-2016
Publisher: American Chemical Society (ACS)
Date: 13-05-2019
Abstract: Block copolymers are versatile building blocks for the self-assembly of functional nanostructures in bulk and solution. While spheres, cylinders, and bilayer sheets are thermodynamically preferred shapes and frequently observed, ring-shaped nanoparticles are more challenging to realize due to energetic penalties that originate from their anisotropic curvature. Today, a handful of concepts exist that produce core-shell nanorings, while more complex ( e. g., patchy) nanorings are currently out of reach and have only been predicted theoretically. Here, we demonstrate that confinement assembly of properly designed ABC triblock terpolymers is a general route to synthesize Janus nanorings in high purity. The triblock terpolymer self-assembles in the spherical confinement of nanoemulsion droplets into prolate ellipsoidal microparticles with an axially stacked lamellar-ring ( lr)-morphology. We clarified and visualized this complex, yet well-ordered, morphology with transmission electron tomography. Blocks A and C formed stacks of lamellae with the B microdomain sandwiched in-between as nanorings. Cross-linking of the B-rings allowed disassembly of the microparticles into Janus nanorings carrying two strictly separated polymer brushes of A and C on the top and bottom. Decreasing the B volume leads to Janus spheres and rods, while an increase of B results in perforated and filled Janus disks. The confinement assembly of ABC triblock terpolymers is a general process that can be extended to other block chemistries and will allow to synthesize a large variety of complex micro- and nanoparticles that inspire studies in self-assembly, interfacial stabilization, colloidal packing, and nanomedicine.
Publisher: Wiley
Date: 26-04-2021
Abstract: The use of labile covalent bonds such as oximes and acetals for their application in the synthesis, and controlled triggered deconstruction, of molecular polymer brushes (MPBs) is reported. Macromonomers (MMs) are produced via reversible addition‐fragmentation chain transfer (RAFT) polymerization using chain transfer agents (CTAs) featuring customized labile moieties. Ring‐opening metathesis polymerization (ROMP) of the MMs using the grafting‐through approach produced MPBs in which the cleavable CTA is incorporated along the backbone, between the brush mainchain and its side chains. Degradation (i.e., the detachment of side chains) of the brush is possible through exposure to an acid stimulus. Especially, ketoxime, solketal, and ethoxyethyl (EE) acetal‐based motifs demonstrate excellent orthogonality to the polymerization protocols. This study highlights how polymer architectures can be built from, and reverted to, single polymer chains by using well‐designed CTAs in a straight‐forward approach.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7PY01814B
Abstract: Precisely grafted polymer brushes on cellulose nanocrystals guide the formation of silica and yield uniform CNC-based hybrid nanomaterials which are subsequently used in the fabrication of hollow and highly porous silica nanorods.
Publisher: Wiley
Date: 02-10-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1PY01581H
Abstract: In this Perspective, we outline advances and challenges in controlling the structure of polymers at various size regimes in the context of structural features such as molecular weight distribution, end groups, architecture, composition and sequence.
Publisher: American Chemical Society (ACS)
Date: 23-11-2020
Publisher: American Chemical Society (ACS)
Date: 13-03-2017
DOI: 10.1021/JACS.6B11302
Abstract: Peptides perform a erse range of physiologically important functions. The formulation of nanoparticles directly from functional peptides would therefore offer a versatile and robust platform to produce highly functional therapeutics. Herein, we engineered proapoptotic peptide nanoparticles from mitochondria-disrupting KLAK peptides using a template-assisted approach. The nanoparticles were designed to disassemble into free native peptides via the traceless cleavage of disulfide-based cross-linkers. Furthermore, the cytotoxicity of the nanoparticles was tuned by controlling the kinetics of disulfide bond cleavage, and the rate of regeneration of the native peptide from the precursor species. In addition, a small molecule drug (i.e., doxorubicin hydrochloride) was loaded into the nanoparticles to confer synergistic cytotoxic activity, further highlighting the potential application of KLAK particles in therapeutic delivery.
Publisher: American Chemical Society (ACS)
Date: 24-09-2018
Publisher: Wiley
Date: 09-01-2019
Abstract: The continuous amalgamation of photocatalysis into existing reversible deactivation radical polymerisation (RDRP) processes has initiated a rapidly propagating area of polymer research in recent years. We introduce bismuth oxide (Bi
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CC00447D
Abstract: The passive tumour targeting and extravasation performance of PEGMA-based cylindrical polymer brushes was investigated, including their behaviour upon changes to their aspect ratio.
Publisher: Wiley
Date: 19-04-2021
Abstract: Cylindrical polymer brushes (CPBs) are macromolecules with nanoparticle proportions. Their modular synthesis enables tailoring of their chemical composition as well as the dialing‐up of overall dimensions and physicochemical properties. In this study, two rod‐like poly[(ethylene glycol) methyl ether methacrylate] (PEGMA)‐based CPBs with varying stiffness but otherwise comparable features and functionality, are synthesized. Differences in particle stiffness are assessed using small angle neutron scattering (SANS). It is observed that the fate of the two CPBs within cells is distinctly different. Stiffer CPBs seem to gravitate toward the mitochondria, whereas CPBs with reduced stiffness are present in different intracellular vesicles.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6PY00635C
Abstract: The synthesis of new, highly functional and dynamic polymeric materials has risen dramatically since the introduction of click chemistry in 2001.
Publisher: Wiley
Date: 14-05-2018
Abstract: Polymer science is rapidly advancing towards the precise construction of synthetic macromolecules of formidable complexity. Beyond the impressive advances in control over polymer composition and uniformity enabled by the living polymerisation revolution, the introduction of compartmentalisation within polymer architectures can elevate their functionality beyond that of their constituent parts, thus offering immense potential for the production of tailor-made nanomaterials. In this Minireview, we discuss synthetic routes to complex molecular brushes with discrete chemical compartments and highlight their potential in the development of advanced materials with applications in nanofabrication, optics and functional materials.
Publisher: American Chemical Society (ACS)
Date: 22-02-2013
DOI: 10.1021/NN3054347
Abstract: A tapping-mode AFM investigation of core-shell cylindrical polymer brushes (CPBs) on mica shows that they can be ruptured upon spin-coating. Three different CPBs were synthesized, having a methacrylate backbone, carrying branches of poly[oligo(ethylene glycol)methacrylate] (POEGMA), POEGMA-block-poly[2-(dimethylamino)ethyl methacrylate] (POEGMA-b-PDMAEMA), and POEGMA-block-poly[2-(methacryloyloxy)ethyl trimethylammoniumiodide] (POEGMA-b-PMETAI). The polymer backbone of core-shell CPB with POEGMA-b-PDMAEMA or POEGMA-b-PMETAI branches is ruptured upon drying on a mica surface, while they are stable in aqueous solution. We propose that the scission behavior is induced by Coulomb interactions between PDMAEMA or PMETAI corona and the solid surface and that this interaction is stronger than one or more carbon-carbon single bonds. We control this scission behavior by tuning the surface interactions through switching the surface nature, varying pH, or adding multivalent counterions. Our study demonstrates that core-shell CPB serves as a template to directly compare the weak intermolecular forces with the strong carbon-carbon covalent bonds.
Publisher: Wiley
Date: 30-09-2016
Abstract: Materials assembled by coordination interactions between naturally abundant polyphenols and metals are of interest for a wide range of applications, including crystallization, catalysis, and drug delivery. Such an interest has led to the development of thin films with tunable, dynamic properties, however, creating bulk materials remains a challenge. Reported here is a class of metallogels formed by direct gelation between inexpensive, naturally abundant tannic acid and group(IV) metal ions. The metallogels exhibit erse properties, including self-healing and transparency, and can be doped with various materials by in situ co-gelation. The robustness and flexibility, combined with the ease, low cost, and scalability of the coordination-driven assembly process make these metallogels potential candidates for chemical, biomedical, and environmental applications.
Publisher: Wiley
Date: 16-09-2020
Abstract: The fabrication of macromolecular architectures with high aspect ratio and well‐defined internal and external morphologies remains a challenge. The combination of template chemistry and self‐assembly concepts to construct peculiar polymer architectures via a bottom‐up approach is an emerging approach. In this study, a cylindrical template—namely a core–shell molecular polymer brush—and linear diblock copolymers (DBCP) associate to produce high aspect ratio polymer particles via interpolyelectrolyte complexation. Induced, morphological changes are studied using cryogenic transmission electron and atomic force microscopy, while the complexation is further followed by isothermal titration calorimetry and ξ‐potential measurements. Depending on the nature of the complexing DBCP, distinct morphological differences can be achieved. While polymers with a non‐ionic block lead to internal compartmentalization, polymers featuring zwitterionic domains lead to a wrapping of the brush template.
Location: No location found
Location: Germany
Start Date: 2018
End Date: 12-2020
Amount: $386,500.00
Funder: Australian Research Council
View Funded ActivityStart Date: 02-2021
End Date: 07-2025
Amount: $909,654.00
Funder: Australian Research Council
View Funded ActivityStart Date: 10-2022
End Date: 10-2025
Amount: $449,000.00
Funder: Australian Research Council
View Funded Activity