Chemical and Biomolecular Engineering - Research Publications

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    Fenton-RAFT Polymerization: An "On-Demand" Chain-Growth Method
    Reyhani, A ; McKenzie, TG ; Ranji-Burachaloo, H ; Fu, Q ; Qiao, GG (WILEY-V C H VERLAG GMBH, 2017-05-29)
    Fine control over the architecture and/or microstructure of synthetic polymers is fast becoming a reality owing to the development of efficient and versatile polymerization techniques and conjugation reactions. However, the transition of these syntheses to automated, programmable, and high-throughput operating systems is a challenging step needed to translate the vast potential of precision polymers into machine-programmable polymers for biological and functional applications. Chain-growth polymerizations are particularly appealing for their ability to form structurally and chemically well-defined macromolecules through living/controlled polymerization techniques. Even using the latest polymerization technologies, the macromolecular engineering of complex functional materials often requires multi-step syntheses and purification of intermediates, and results in sub-optimal yields. To develop a proof-of-concept of a framework polymerization technique that is readily amenable to automation requires several key characteristics. In this study, a new approach is described that is believed to meet these requirements, thus opening avenues toward automated polymer synthesis.
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    Antifogging Surface Facilitated by Nanoscale Coatings with Controllable Hydrophobicity and Cross-Linking Density
    Nam, E ; Wong, EHH ; Tan, S ; Fu, Q ; Blencowe, A ; Qiao, GG (WILEY-V C H VERLAG GMBH, 2017-01)
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    Sono‐RAFT Polymerization in Aqueous Medium
    McKenzie, TG ; Colombo, E ; Fu, Q ; Ashokkumar, M ; Qiao, GG (Wiley, 2017-09-25)
    The ultrasonic irradiation of aqueous solution is demonstrated to be a suitable source of initiating radicals for a controlled radical polymerization when conducted in the presence of a thiocarbonylthio-containing reversible addition–fragmentation chain transfer (RAFT) agent. This allows for a highly “green” method of externally regulated/controlled polymerization with a potentially broad scope for polymerizable monomers and/or polymer structures.
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    Sono-RAFT Polymerization in Aqueous Medium
    McKenzie, TG ; Colombo, E ; Fu, Q ; Ashokkumar, M ; Qiao, GG (WILEY-V C H VERLAG GMBH, 2017-09-25)
    The ultrasonic irradiation of aqueous solution is demonstrated to be a suitable source of initiating radicals for a controlled radical polymerization when conducted in the presence of a thiocarbonylthio-containing reversible addition-fragmentation chain transfer (RAFT) agent. This allows for a highly "green" method of externally regulated/controlled polymerization with a potentially broad scope for polymerizable monomers and/or polymer structures.
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    An Exciting Time for Polymer Chemists in Australia
    Boyer, C ; Qiao, G (John Wiley & Sons, Inc., 2019-09-15)
    Over the last 50 years, Australian researchers have made significant contributions to polymer science. Australian scientists have participated in the discovery of many polymerization techniques such as nitroxide‐mediated polymerization (NMP), addition‐fragmentation polymerization (AFT), and the well‐known Reversible Addition‐Fragmentation Chain Transfer polymerization (RAFT), as well as the successful commercialization of products utilizing polymers, most notably the plastic banknote. These contributions have been led by the Australian scientists working at the Commonwealth Scientific and Industrial Research Organisation (CSIRO) and Australian universities. Despite previous attempts by other reserve banks in different countries, the Reserve Bank of Australia introduced the first plastic banknote developed by the CSIRO in collaboration with Note Printing Australia.
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    Fenton-Chemistry-Mediated Radical Polymerization
    Reyhani, A ; McKenzie, TG ; Fu, Q ; Qiao, GG (Wiley, 2019-09-01)
    In this review, the power of a classical chemical reaction, the Fenton reaction for initiating radical polymerizations, is demonstrated. The reaction between the Fenton reagents (i.e., Fe2+ and H2O2) generates highly reactive hydroxyl radicals, which can act as radical initiators for the polymerization of vinyl monomers. Since the Fenton reaction is fast, easy to set up, cheap, and biocompatible, this unique chemistry is widely employed in various polymer synthesis studies via free radical polymerization or reversible addition–fragmentation chain transfer polymerization, and is utilized in a wide range of applications, such as the fabrication of biomaterials, hydrogels, and core‐shell particles. Biologically activated Fenton‐mediated radical polymerization, which can be performed in aerobic environments, are particularly useful for applications in biomedical systems.
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    Ultrasound and Sonochemistry for Radical Polymerization: Sound Synthesis
    McKenzie, TG ; Karimi, F ; Ashokkumar, M ; Qiao, GG (WILEY-V C H VERLAG GMBH, 2019-04-11)
    The use of ultrasound as an external stimulus for promoting polymerization reactions has received increasing attention in recent years. In this Review article, the fundamental processes that can lead to either the homolytic cleavage of polymer chains, or the sonolysis of solvent (or other) small molecules, under the application of ultrasound are described. These reactions promote the production of reactive radicals, which can be utilized in chain-growth radical polymerizations under the right conditions. A full historical overview of the development of ultrasound-assisted radical polymerization is provided, with special attention given to the recently described systems that are "controlled" by methods of reversible (radical) deactivation. Perspectives are shared on what challenges still remain in polymer sonochemistry, as well as new areas that are yet to be explored.
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    Synthesis of ultra-high molecular weight polymers by controlled production of initiating radicals
    Reyhani, A ; Allison-Logan, S ; Ranji-Burachaloo, H ; McKenzie, TG ; Bryant, G ; Qiao, GG (John Wiley & Sons, Inc., 2019-09-15)
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    Blood‐Catalyzed RAFT Polymerization
    Reyhani, A ; Nothling, MD ; Ranji‐Burachaloo, H ; McKenzie, TG ; Fu, Q ; Tan, S ; Bryant, G ; Qiao, GG (Wiley, 2018-08-06)
    Abstract The use of hemoglobin (Hb) contained within red blood cells to drive a controlled radical polymerization via a reversible addition‐fragmentation chain transfer (RAFT) process is reported for the first time. No pre‐treatment of the Hb or cells was required prior to their use as polymerization catalysts, indicating the potential for synthetic engineering in complex biological microenvironments without the need for ex vivo techniques. Owing to the naturally occurring prevalence of the reagents employed in the catalytic system (Hb and hydrogen peroxide), this approach may facilitate the development of new strategies for in vivo cell engineering with synthetic macromolecules.
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    MOF Scaffold for a High‐Performance Mixed‐Matrix Membrane
    Xie, K ; Fu, Q ; Webley, PA ; Qiao, GG (Wiley, 2018-07-09)
    Abstract A novel composite membrane consisting of an interconnected MOF scaffold coated with cross‐linked poly(ethylene glycol) (PEG) has been developed. As a result of its unique structure, the membrane shows an exceptional 18‐fold permeability enhancement as compared to pristine PEG membranes, without compromising the selectivity. This performance is unattainable with current mixed‐matrix membranes (MMMs). Our optimized membrane has a permeability of 2700 Barrer with a CO2/N2 selectivity of 35, which surpasses the latest Robeson upper bound.