ORCID Profile
0000-0002-5419-7561
Current Organisation
Queensland University of Technology
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In Research Link Australia (RLA), "Research Topics" refer to ANZSRC FOR and SEO codes. These topics are either sourced from ANZSRC FOR and SEO codes listed in researchers' related grants or generated by a large language model (LLM) based on their publications.
Macromolecular and Materials Chemistry | Synthesis of Materials | Macromolecular and Materials Chemistry not elsewhere classified | Polymerisation Mechanisms | Chemical Characterisation of Materials
Expanding Knowledge in the Chemical Sciences | Organic Industrial Chemicals (excl. Resins, Rubber and Plastics) | Plastics in Primary Forms | Polymeric Materials (e.g. Paints) | Aerospace Transport not elsewhere classified |
Publisher: Wiley
Date: 19-03-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0PY01045F
Abstract: The synthesis of single chain nanoparticles (SCNPs) is a vibrant field in macromolecular science. However, to achieve an in-depth understanding of the nature of intramolecular polymer folding, a step-change in the methodologies for SCNP analysis is required.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C2CC37157J
Abstract: We report here the synthesis of a novel electroactive polyolefin and demonstrate through a combination of SEC-MALS and DLS how this type of functional polymer can be folded in a controlled fashion from an expanded coil to a tightly wound globule using sequentially activated noncovalent and covalent intra-chain interactions.
Publisher: Wiley
Date: 29-03-2023
Abstract: A photoresist—based on a light‐stabilized dynamic material driven by an out‐of‐equilibrium photo‐Diels–Alder reaction of triazolinediones with naphthalenes—whose ability to intrinsically degrade postprinting can be tuned by a simple adjustment of laser intensity during 3D laser lithography is introduced. The resist's ability to form stable networks under green light irradiation that degrade in the dark is transformed into a tunable degradable 3D printing material platform. In‐depth characterization of the printed microstructures via atomic force microscopy before and during degradation reveals the high dependency of the final structures’ properties on the writing parameters. Upon identifying the ideal writing parameters and their effect on the network structure, it is possible to selectively toggle between stable and fully degradable structures. This simplifies the direct laser writing manufacturing process of multifunctional materials significantly, which typically requires the use of separate resists and consecutive writing efforts to achieve degradable and nondegradable material sections.
Publisher: American Chemical Society (ACS)
Date: 15-09-2016
DOI: 10.1021/ACS.INORGCHEM.6B01113
Abstract: Porphyrin-cored polymer nanoparticles (PCPNs) were synthesized and characterized to investigate their utility as heme protein models. Created using collapsible heme-centered star polymers containing photodimerizable anthracene units, these systems afford model heme cofactors buried within hydrophobic, macromolecular environments. Spectroscopic interrogations demonstrate that PCPNs display redox and ligand-binding reactivity similar to that of native systems and thus are potential candidates for modeling biological heme iron coordination.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7CC00711F
Abstract: We report a visible light responsive moiety capable of generating highly reactive thioaldehydes.
Publisher: American Chemical Society (ACS)
Date: 25-08-2020
DOI: 10.26434/CHEMRXIV.12854636.V1
Abstract: The formation of single chain nanoparticles (SCNPs) is typically characterized by a shift towards higher elution volumes in SEC due to size decrease upon folding. However, a step-change in SCNP analysis is required for understanding of the nature of intramolecular SCNP folding. Herein, we exploit a unique combination of SANS, 19F NMR spectroscopy, and multidetection SEC to generate a systematic view of the folded morphology of poly(butyl acrylate) based-SCNPs as a function of their reactive group density and molar mass. In addition to detailed morphological insights, we establish that the primary factor dictating the compaction of SCNPs is their reactive group density, which is ineffective below 5 mol%, reaching maximum compaction close to 30 mol%. Above 20 kDa the molar mass of the precursor polymers has a minor impact on how an SCNP compacts.
Publisher: American Chemical Society (ACS)
Date: 10-10-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY01278K
Abstract: We provide the results of a critical literature survey on the reported sizes of single chain polymer nanoparticles (SCNPs) employing different techniques.
Publisher: Wiley
Date: 24-04-2019
Abstract: We report light-induced reactions in a two-chromophore system capable of sequence-independent λ-orthogonal reactivity relying solely on the choice of wavelength and solvent. In a solution of water and acetonitrile, LED irradiation at λ
Publisher: American Chemical Society (ACS)
Date: 11-07-2018
Publisher: Wiley
Date: 26-04-2023
Abstract: We introduce a single‐chain nanoparticle (SCNP) system capable of catalyzing the photooxidation of nonpolar alkenes up to three times more efficiently than an equivalent small‐molecule photosensitizer at an identical concentration. Specifically, we construct a polymer chain constituted of poly(ethylene glycol) methyl ether methacrylate and glycidyl methacrylate which we compact via multifunctional thiol‐epoxide ligation and functionalize with Rose Bengal ( RB ) in a one pot reaction, affording SCNPs with a hydrophilic shell and hydrophobic photocatalytic regions. Photooxidation of the internal alkene in oleic acid proceeds under green light. RB confined within the SCNP is three times more effective for nonpolar alkenes than free RB in solution, which we hypothesize is due to the spatial proximity of the photosensitizing units to the substrate in the hydrophobic region. Our approach demonstrates that SCNP based catalysts can afford enhanced photocatalysis via confinement effects in a homogeneous reaction environment.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC90087H
Abstract: We explore and comment on a key development using advanced mass spectrometric methods coupled with advanced algorithmic learning that can assist in analysing complex copolymers.
Publisher: American Chemical Society (ACS)
Date: 27-12-2016
DOI: 10.1021/JACS.6B10952
Abstract: Herein, we introduce the first approach to map single-chain nanoparticle (SCNP) folding via high-resolution electrospray ionization mass spectrometry (ESI MS) coupled with size exclusion chromatography. For the first time, the successful collapse of polymeric chains into SCNPs is imaged by characteristic mass changes, providing detailed mechanistic information regarding the folding mechanism. As SCNP system we employed methyl methacrylate (MMA) statistically copolymerized with glycidyl methacrylate (GMA), resulting in p(MMA-stat-GMA), subsequently collapsed by using B(C
Publisher: Wiley
Date: 12-10-2020
Publisher: American Chemical Society (ACS)
Date: 25-03-2022
DOI: 10.1021/ACS.JPCLETT.2C00386
Abstract: The appeal of metal halide perovskite solar cells (PSCs) has been widely demonstrated in the field of photovoltaic technology. On account of the excellent optical and electrical properties, as well as compatibility with flexible substrates, the PSCs also hold the highest record of specific power for lightweight solar cell devices, suggesting excellent promise in space applications. Hence, there is increasing interest in the performance of PSCs in space environments where radiation beams and thermal cycling can cause extreme stress on the devices. In this Perspective, we provide a brief summary of the research on PSCs for space applications. The radiation tolerance and thermal stability of PSCs and the fundamental mechanisms are discussed and analyzed. Key challenges facing PSC technology toward future space applications are demonstrated. This Perspective features the prospect of PSCs as the next frontier in space PV technology.
Publisher: American Chemical Society (ACS)
Date: 25-08-2020
DOI: 10.26434/CHEMRXIV.12854636
Abstract: The formation of single chain nanoparticles (SCNPs) is typically characterized by a shift towards higher elution volumes in SEC due to size decrease upon folding. However, a step-change in SCNP analysis is required for understanding of the nature of intramolecular SCNP folding. Herein, we exploit a unique combination of SANS, 19F NMR spectroscopy, and multidetection SEC to generate a systematic view of the folded morphology of poly(butyl acrylate) based-SCNPs as a function of their reactive group density and molar mass. In addition to detailed morphological insights, we establish that the primary factor dictating the compaction of SCNPs is their reactive group density, which is ineffective below 5 mol%, reaching maximum compaction close to 30 mol%. Above 20 kDa the molar mass of the precursor polymers has a minor impact on how an SCNP compacts.
Publisher: American Chemical Society (ACS)
Date: 20-10-2020
DOI: 10.1021/ACSMACROLETT.0C00519
Abstract: The intramolecular chain collapse of linear precursors with systematic variation of molar mass and ligation group density (5, 15, and 30 mol %) into single-chain nanoparticles (SCNPs) was studied by two different separation approaches. The efficiency of size exclusion chromatography with quadruple detection (SEC-D4) was compared to asymmetrical field flow fractionation hyphenated to quintuple detection (AF4-D5) in organic solvent. The application of the unique combination of advanced detection to different separation principles opens up the opportunity to critically evaluate the determination of molar masses and different types of radii for an in-depth understanding of the structural properties affected by the internal folding process. This is achieved by a detailed comparison of assets, drawbacks, and limitations of these approaches based on the systematical screening of different chain lengths and sizes of the precursors and the SCNPs. Furthermore, an alternative strategy for quantitative determination of intramolecular ligation density by a combination of AF4 and UV detection is introduced.
Publisher: Elsevier BV
Date: 08-2022
Publisher: American Chemical Society (ACS)
Date: 15-07-2015
Publisher: Wiley
Date: 30-10-2013
Abstract: An efficient route to architecturally defined, sub-20 nm soft nanoparticles fabricated from single polymer chains via intramolecular photodimerization of pendant anthracene units is presented. Photodimerization is confirmed by the disappearance of the characteristic anthracene π-π* absorption peak at ≈ 360 nm measured by UV-vis spectroscopy. Size exclusion chromatography (SEC) with UV, multi-angle light scattering (MALS), and viscometric detection confirms that as photodimers form, the chains fold to form nanoparticles, demonstrated by shifts in the SEC traces to longer retention times as a function of increased irradiation time. These shifts indicate a reduction in hydrodynamic radius, corroborated and quantified by viscometric data. MALS detector traces reveal the presence of a small amount of chain-chain coupling during this process, but confirm that this is primarily a single-chain phenomenon. Electron microscopy provides visual confirmation of nanoparticle formation.
Publisher: Wiley
Date: 24-05-2018
Abstract: A self-reporting, profluorescent, visible light-induced release system is introduced. Fluorescence activation is enabled by a mild remote trigger signal that can be monitored with the naked-eye in real time. The light-responsive spin-silenced polymer is synthesized via an Ugi post-polymerization modification incorporating paramagnetic nitroxides and a light cleavable fluorophore moiety.
Publisher: Wiley
Date: 26-04-2023
Abstract: Wir stellen ein Einzelkettennanopartikel (SCNP)‐System vor, welches bei identischer Konzentration die Photooxidation unpolarer Alkene bis zu dreimal effizienter katalysieren kann als ein äquivalenter niedermolekularer Photosensibilisator. Konkret haben wir SCNPs basierend auf Poly(ethylenglykol)methylethermethacrylat und Glycidylmethacrylat entwickelt, welches wir über multifunktionelle Thiol‐Epoxid‐Verknüpfungen in Kombination mit der Funktionalisierung mit Bengalrosa (RB) in einer Eintopfreaktion falten. Die SCNPs weisen sowohl eine hydrophile Hülle als auch hydrophobe photokatalytische Regionen auf. Die Photooxidation des innenliegenden Alkens der Ölsäure verläuft unter Einstrahlung von grünem Licht. Kovalent an die SCNPs gebundenes RB ist dreimal sensitiver gegenüber unpolaren Alkene als freies RB in Lösung. Dies ist unserer Hypothese nach auf die räumliche Nähe der photosensibilisierenden Gruppen zum Substrat in der hydrophoben Region zurückzuführen. Unser Ansatz zeigt, dass SCNP‐basierte Katalysatoren eine verbesserte Photokatalyse durch Einschränkungseffekte (confinement effects) in einer homogenen Reaktionsumgebung ermöglichen können.
Publisher: Wiley
Date: 29-10-2021
Abstract: Melt electrowriting (MEW) has been widely used to process polycaprolactone (PCL) into highly ordered microfiber scaffolds with controllable architecture and geometry. However, the integrity of PCL during specific processes involved in routine MEW scaffold development has not yet been thoroughly investigated. This study investigates the impact of MEW processing on PCL following exposure to high temperatures required for melt extrusion as well as atmospheric plasma, a widely used surface treatment for improving MEW scaffold hydrophilicity. The change in polymer molecular weight and melt temperature is characterized, in comparing unprocessed and processed s les, in addition to analysis of the mechanical and surface properties of the scaffolds. No significant difference in the molecular weight or mechanical properties of the PCL scaffolds is evident following 5 days of cyclic heating to 90 °C. Exposure to plasma for up to 5 min significantly increased hydrophilicity and surface adhesion force, characterized via contact angle and atomic force microscope, however, significant polymer degradation occurred evidenced by increased brittleness of the scaffolds. This study demonstrates the degradation of PCL following fabrication via MEW and surface treatment to guide the optimization of scaffold development for subsequent applications in tissue engineering and biofabrication.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5PY00265F
Abstract: The intra-chain radical polymerization of pendant methacryloyl decorated poly(norbornene) imides is a viable route to single-chain nanoparticles, however this process is complicated by adventitious molecular oxygen.
Publisher: Springer Science and Business Media LLC
Date: 26-02-2014
Publisher: Elsevier BV
Date: 2020
Publisher: Wiley
Date: 26-06-2022
Abstract: To advance the applications of direct laser writing (DLW), adaptability of the printed structure is critical, prompting a shift toward printing structures that are comprised of different materials, and/or can be partially or fully erased on demand. However, most structures that contain these features are often printed by complex processes or require harsh developing techniques. Herein, a unique photoresist for DLW is introduced that is capable of printing 3D microstructures that can be erased by exposure to darkness. Specifically, microstructures based on light‐stabilized dynamic materials are fabricated that remain stable when continously irradiated with green light, but degrade once the light source is switched off. The degradation and light stabilization properties of the printed materials are analyzed in‐depth by time‐lapse scanning electron microscopy. It is demonstrated that these resists can be used to impart responsive behavior onto the printed structure, and –critically– as a temporary locking mechanism to control the release of moving structural features.
Publisher: American Chemical Society (ACS)
Date: 15-05-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2PY20308A
Publisher: American Chemical Society (ACS)
Date: 09-05-2018
Publisher: Wiley
Date: 24-04-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4PY01217H
Abstract: In this review we outline the various methods that have been explored to synthesize architecturally defined nanoparticles from discrete polymer chains, summarize the methods of characterization that are required to prove their formation and probe their morphology, and introduce a number of potential applications.
Publisher: Wiley
Date: 2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1CC02984C
Abstract: We introduce a four component Passerini polymerization utilizing sterically bulky isocyanide monomers.
Publisher: Wiley
Date: 20-10-2015
DOI: 10.1002/POLA.27942
Publisher: Wiley
Date: 19-03-2019
Abstract: Herein, we introduce an additive-free visible-light-induced Passerini multicomponent polymerization (MCP) for the generation of high molar mass chains. In place of classical aldehydes (or ketones), highly reactive, in situ photogenerated thioaldehydes are exploited along with isocyanides and carboxylic acids. Prone to side reactions, the thioaldehyde moieties create a complex reaction environment which can be tamed by optimizing the synthetic conditions utilizing stochastic reaction path analysis, highlighting the potential of semi-batch procedures. Once the complex MCP environment is understood, step-growth polymers can be synthesized under mild reaction conditions which-after a Mumm rearrangement-result in the incorporation of thioester moieties directly into the polymer backbone, leading to soft matter materials that can be degraded by straightforward aminolysis or chain expanded by thiirane insertion.
Start Date: 03-2020
End Date: 12-2024
Amount: $415,498.00
Funder: Australian Research Council
View Funded ActivityStart Date: 06-2022
End Date: 06-2025
Amount: $435,588.00
Funder: Australian Research Council
View Funded Activity