ORCID Profile
0000-0002-7504-5508
Current Organisation
Flinders University
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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.
Organic Chemical Synthesis | Organic Chemistry | Macromolecular and Materials Chemistry | Synthesis of Materials | Macromolecular materials | Organic chemical synthesis | Organic Green Chemistry | Proteins and Peptides | Physical Organic Chemistry | Macromolecular and materials chemistry | Optical properties of materials | Characterisation of Biological Macromolecules | Medicinal and Biomolecular Chemistry | Colloid and Surface Chemistry | Inorganic Green Chemistry | Biologically Active Molecules | Structural Chemistry and Spectroscopy | Macromolecular and materials chemistry not elsewhere classified | Chemical engineering | Analytical Biochemistry | Electrochemical energy storage and conversion
Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in the Biological Sciences | Environmentally Sustainable Mineral Resource Activities not elsewhere classified | Chemical Fertilisers | Organic Industrial Chemicals (excl. Resins, Rubber and Plastics) | Environmentally Sustainable Manufacturing not elsewhere classified | Expanding Knowledge in the Medical and Health Sciences | Rehabilitation of Degraded Coastal and Estuarine Environments | Management of Solid Waste from Manufacturing Activities |
Publisher: Springer Science and Business Media LLC
Date: 13-07-2023
DOI: 10.1007/S11154-023-09823-3
Abstract: Background and aims : Bariatric surgery is the most effective treatment in in iduals with obesity to achieve remission of type 2 diabetes. Post-bariatric surgery hypoglycaemia occurs frequently, and management remains suboptimal, because of a poor understanding of the underlying pathophysiology. The glucoregulatory hormone responses to nutrients in in iduals with and without post-bariatric surgery hypoglycaemia have not been systematically examined. Materials and methods : The study protocol was prospectively registered with PROSPERO. PubMed, EMBASE, Web of Science and the Cochrane databases were searched for publications between January 1990 and November 2021 using MeSH terms related to post-bariatric surgery hypoglycaemia. Studies were included if they evaluated in iduals with post-bariatric surgery hypoglycaemia and included measurements of plasma glucagon-like peptide-1 (GLP-1), glucose-dependent insulinotropic polypeptide (GIP), insulin, C-peptide and/or glucagon concentrations following an ingested nutrient load. Glycated haemoglobin (HbA 1c ) was also evaluated. A random-effects meta-analysis was performed, and Hedges’ g (standardised mean difference) and 95% confidence intervals were reported for all outcomes where sufficient studies were available. The τ 2 estimate and I 2 statistic were used as tests for heterogeneity and a funnel plot with the Egger regression-based test was used to evaluate for publication bias. Results : From 377 identified publications, 12 were included in the analysis. In all 12 studies, the type of bariatric surgery was Roux-en-Y gastric bypass (RYGB). Comparing in iduals with and without post-bariatric surgery hypoglycaemia following an ingested nutrient load, the standardised mean difference in peak GLP-1 was 0.57 (95% CI, 0.32, 0.82), peak GIP 0.05 (-0.26, 0.36), peak insulin 0.84 (0.44, 1.23), peak C-peptide 0.69 (0.28, 1.1) and peak glucagon 0.05 (-0.26, 0.36). HbA 1c was less in in iduals with hypoglycaemia − 0.40 (-0.67, -0.12). There was no evidence of substantial heterogeneity in any outcome except for peak insulin: τ 2 = 0.2, I 2 = 54.3. No publication bias was evident. Conclusion : Following RYGB, postprandial peak plasma GLP-1, insulin and C-peptide concentrations are greater in in iduals with post-bariatric surgery hypoglycaemia, while HbA 1c is less. These observations support the concept that antagonism of GLP-1 would prove beneficial in the management of in iduals with hypoglycaemia following RYGB. PROSPERO Registration Number: CRD42021287515.
Publisher: Wiley
Date: 10-03-2021
Abstract: An insulating composite was made from the sustainable building blocks wool, sulfur, and canola oil. In the first stage of the synthesis, inverse vulcanization was used to make a polysulfide polymer from the canola oil triglyceride and sulfur. This polymerization benefits from complete atom economy. In the second stage, the powdered polymer was mixed with wool, coating the fibers through electrostatic attraction. The polymer and wool mixture were then compressed with mild heating to provoke S−S metathesis in the polymer, which locks the wool in the polymer matrix. The wool fibers imparted tensile strength, insulating properties, and reduced the flammability of the composite. All building blocks are sustainable or derived from waste and the composite is a promising lead on next‐generation insulation for energy conservation.
Publisher: American Chemical Society (ACS)
Date: 18-02-2022
Publisher: American Chemical Society (ACS)
Date: 07-2022
Publisher: American Chemical Society (ACS)
Date: 23-02-2018
DOI: 10.1021/JACS.7B12874
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7GC03352D
Abstract: Continuous flow vortex microfluidics is effective in overcoming limitations in using oxygen, hydrogen peroxide and bleach as oxidants.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3RA41231H
Publisher: Wiley
Date: 13-01-2012
Publisher: American Chemical Society (ACS)
Date: 31-10-2022
DOI: 10.26434/CHEMRXIV-2022-BZZD3
Abstract: With increasing use of infrared imaging in medical diagnostics, military and civilian surveillance, and navigation of autonomous vehicles, there is a need for low-cost alternatives to traditional materials used in infrared optics such as germanium. Sulfur-rich copolymers hold promise, as they are made from low-cost feedstocks and have a high refractive index. In this report, cyclopentadiene was copolymerized with sulfur to provide a plastic with the highest long-wave infrared transparency reported to date for this class of materials. Diverse lens architectures were accessible through melt casting or reactive injection molding. The featured copolymer was black, which enabled its use as an infrared-transparent blind for protection of thermal imaging equipment and clandestine surveillance. These findings portend expanded use of sulfur copolymers in infrared optics.
Publisher: American Chemical Society (ACS)
Date: 07-2008
DOI: 10.1021/JA8026168
Abstract: Allyl sulfides undergo efficient cross-metathesis in aqueous media with Hoveyda-Grubbs second generation catalyst 1. The high reactivity of allyl sulfides in cross-metathesis was exploited in the first ex les of cross-metathesis on a protein surface. S-Allylcysteine was incorporated chemically into the protein, providing the requisite allyl sulfide handle. Preliminary efforts to genetically incorporate S-allylcysteine into proteins are also reported.
Publisher: Wiley
Date: 08-07-2019
Abstract: Sulfur is an underused by-product of the petrochemicals industry. Recent research into inverse vulcanization has shown how this excess sulfur can be transformed into functional polymers, by stabilization with organic crosslinkers. For these interesting new materials to realize their potential for applications, more understanding and control of their physical properties is needed. Here we report four new terpolymers prepared from sulfur and two distinct alkene monomers that can be predictively tuned in glass transition, molecular weight, solubility, mechanical properties, and color.
Publisher: Georg Thieme Verlag KG
Date: 04-2021
DOI: 10.1055/A-1502-2611
Abstract: Inverse vulcanization is a process in which highly abundant and low-cost elemental sulfur is copolymerized with an unsaturated organic molecule such as a polyene. This process has provided a variety of useful materials with high sulfur content—typically 50% or greater in sulfur by mass. These materials have garnered increasing interest in research as sorbents for mercury, due to the high affinity of sulfur for mercury. In this review, the features of mercury sorbents made by inverse vulcanization are presented. Additionally, case studies are provided to illustrate the variety of polymer architectures accessible with this chemistry, the versatility of these materials in mercury remediation, and prospects for industrial use. 1 Introduction 2 Sulfur Polymers by Inverse Vulcanization 3 Sulfur Polymers as Mercury Sorbents 4 Increasing Surface Area to Improve Mercury Uptake 5 Crosslinker Considerations 6 Sorption of Different Forms of Mercury 7 Life-Cycle Management 8 Conclusions and Outlook
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CP01903E
Abstract: Detailed kinetic modelling of mercury uptake for a sulfur-limonene copolymer was undertaken. The effect of pH and salt concentration on mercury sorption, as well as selectivity, was assessed for the first time for this mercury-binding polymer.
Publisher: Springer International Publishing
Date: 2019
Publisher: American Chemical Society (ACS)
Date: 02-08-2023
DOI: 10.26434/CHEMRXIV-2023-VMHTD
Abstract: The emergence of more virulent and epidemic strains of viruses, especially with the current COVID-19 pandemic, makes it more important than ever to improve methods of decontamination. The use of vapour dispersion devices or “foggers” have played a critical role in rapidly applying disinfectants over large areas or complex surfaces to prevent the spread of pathogens. The objective of this study was to evaluate the potential of on-demand production of chlorine species to inactivate human coronaviruses. The commercial prototype disinfection unit was provided by Unipolar Water Technologies. The Unipolar device generates active chlorine species using an electrochemical reaction and dispenses the disinfectant vapour onto surfaces with an aspirator. The minimum effective concentration and exposure time of disinfectant were evaluated on human hepatoma (Huh7) cells using 50% tissue culture infectious dose (TCID50) assay and human coronavirus 229E (HCoV-229E), a surrogate for pathogenic human coronaviruses. We showed that chlorine species generated in the Unipolar device inactivates HCoV-229E at ≥ 400 parts per million active chlorine concentration with a 5 min exposure time. Importantly, no toxic effect was observed on Huh7 cells for any of the active chlorine concentrations and contact times tested.
Publisher: American Chemical Society (ACS)
Date: 22-03-2008
DOI: 10.1021/JA800800P
Abstract: An efficient and robust oxidative elimination of cysteine to dehydroalanine has been discovered. The reaction is induced by O-mesitylenesulfonylhydroxylamine (MSH) and is compatible with methionine. The key elimination has been executed on protein surfaces and allows ready access to different post-translationally modified proteins through conjugate addition of sulfur nucleophiles to dehydroalanine. Treatment of the resulting thioether with MSH results in regeneration of dehydroalanine, allowing a "functional switch" by subsequent addition of a different thiol.
Publisher: Wiley
Date: 23-11-2022
Abstract: A polysulfide terpolymer made from canola oil, dicyclopentadiene, and elemental sulfur is synthesized and evaluated as bulk structural material. The unique polysulfide structure in this material allows the two polymer blocks to be bonded together through amine‐catalyzed SS metathesis. No exogenous adhesive is required: the polysulfide is both the bulk material and the mortar. The strength of the joined polymers is evaluated by a series of shear tests and compared to the bond strength obtained with commercially available superglue. The adhesion obtained via the SS metathesis is stronger in all tests. To improve the mechanical properties of the terpolymer, carbon nanorods and carbon fibers are embedded in the polymer, with the latter leading to nearly a 16‐fold increase in flexural strength. Prospects in sustainable construction are discussed.
Publisher: American Chemical Society (ACS)
Date: 17-05-2023
DOI: 10.1021/JACS.3C03239
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1PY01416A
Abstract: A copolymer made from sulfur and dicyclopentadiene was useful as a mercury sorbent, and also as a protective and repairable coating.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0SC00855A
Abstract: Polymers made by inverse vulcanization can be assembled, repaired, and recycled at room temperature through nucleophile-catalyzed S–S metathesis.
Publisher: Wiley
Date: 20-04-2018
DOI: 10.1002/PEP2.24069
Publisher: American Chemical Society (ACS)
Date: 19-10-2021
DOI: 10.26434/CHEMRXIV-2021-N91H4
Abstract: The reaction between sulfur and dicyclopentadiene was optimised to form a shelf stable and soluble low molecular weight oligomer. After a simple curing process at 140 °C the material was rendered insoluble and resistant to acids and solvents. Taking advantage of the soluble oligomer, a metal surface was coated with the dissolved material which was then cured to show that a copolymer layer can act as a corrosion resistant material. Further, silica gel was coated with the soluble oligomer to test mercury removal applications. Even after curing, the polymer coated silica was an effective mercury sorbent. Additionally, the sorbent was also used to remove mercury form a diesel and water mixture indicating that mercury removal from a mixture of organic and aqueous substances is possible with this system.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1SC00185J
Publisher: American Chemical Society (ACS)
Date: 20-07-2005
DOI: 10.1021/OL051049I
Abstract: Easily prepared allyl phenyl sulfones, capable of introduction of the alkene by electrophilic alpha-substitution, are superior to allyl acetates as substrates for Pd-catalyzed Zn-ene cyclizations, providing C5 or C(4)N rings with cis-1,2-vinyl and -CH(2)Zn substituents. Several ex les, with different methods of substrate preparation, are presented. [reaction: see text]
Publisher: American Chemical Society (ACS)
Date: 25-08-2011
DOI: 10.1021/JO201341Q
Abstract: A highly practical synthesis of enantiopure (-)-α-kainic acid is accomplished in 37% overall yield, using 13 linear steps and a minimum of chromatographic separations via an unprecedented TMSCl-promoted palladium-catalyzed zinc-ene cyclization of an allyl acetate.
Publisher: American Chemical Society (ACS)
Date: 12-05-2011
DOI: 10.1021/AR200056Q
Abstract: Covalent modification can expand a protein's functional capacity. Fluorescent or radioactive labeling, for instance, allows imaging of a protein in real time. Labeling with an affinity probe enables isolation of target proteins and other interacting molecules. At the other end of this functional spectrum, protein structures can be naturally altered by enzymatic action. Protein-protein interactions, genetic regulation, and a range of cellular processes are under the purview of these post-translational modifications. The ability of protein chemists to install these covalent additions selectively has been critical for elucidating their roles in biology. Frequently the transformations must be applied in a site-specific manner, which demands the most selective chemistry. In this Account, we discuss the development and application of such chemistry in our laboratory. A centerpiece of our strategy is a "tag-and-modify" approach, which entails sequential installation of a uniquely reactive chemical group into the protein (the "tag") and the selective or specific modification of this group. The chemical tag can be a natural or unnatural amino acid residue. Of the natural residues, cysteine is the most widely used as a tag. Early work in our program focused on selective disulfide formation in the synthesis of glycoproteins. For certain applications, the susceptibility of disulfides to reduction was a limitation and prompted the development of several methods for the synthesis of more stable thioether modifications. The desulfurization of disulfides and conjugate addition to dehydroalanine are two routes to these modifications. The dehydroalanine tag has since proven useful as a general precursor to many modifications after conjugate addition of various nucleophiles phosphorylated, glycosylated, peptidylated, prenylated, and even mimics of methylated and acetylated lysine-containing proteins are all accessible from dehydroalanine. While cysteine is a useful tag for selective modification, unnatural residues present the opportunity for bio-orthogonal chemistry. Azide-, arylhalide-, alkyne-, and alkene-containing amino acids can be incorporated into proteins genetically and can be specifically modified through various transformations. These transformations often rely on metal catalysis. The Cu-catalyzed azide-alkyne addition, Ru-catalyzed olefin metathesis, and Pd-catalyzed cross-coupling are ex les of such transformations. In the course of adapting these reactions to protein modification, we learned much about the behavior of these reactions in water, and in some cases entirely new catalysts were developed. Through a combination of these bio-orthogonal transformations from the panel of tag-and-modify reactions, multiple and distinct modifications can be installed on protein surfaces. Multiple modifications are common in natural systems, and synthetic access to these proteins has enabled study of their biological role. Throughout these investigations, much has been learned in chemistry and biology. The demands of selective protein modification have revealed many aspects of reaction mechanisms, which in turn have guided the design of reagents and catalysts that allow their successful deployment in water and in biological milieu. With this ability to modify proteins, it is now possible to interrogate biological systems with precision that was not previously possible.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3CC47232A
Abstract: Alginic acid was converted to a variety of ammonium alginate derivatives carrying erse chemical cargo such as analgesics, antibiotics, and enzymes. These functional polymers could be fashioned into nanofibrous mats by electrostatic spinning. The therapeutic payload could be released in functional form by a simple ion exchange mechanism. Prospects in wound healing are discussed.
Publisher: American Chemical Society (ACS)
Date: 04-11-2010
DOI: 10.1021/JA104994D
Abstract: Olefin metathesis has recently emerged as a viable reaction for chemical protein modification. The scope and limitations of olefin metathesis in bioconjugation, however, remain unclear. Herein we report an assessment of various factors that contribute to productive cross-metathesis on protein substrates. Sterics, substrate scope, and linker selection are all considered. It was discovered during this investigation that allyl chalcogenides generally enhance the rate of alkene metathesis reactions. Allyl selenides were found to be exceptionally reactive olefin metathesis substrates, enabling a broad range of protein modifications not previously possible. The principles considered in this report are important not only for expanding the repertoire of bioconjugation but also for the application of olefin metathesis in general synthetic endeavors.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0CC04401F
Abstract: Azide–alkyne cycloadditions in a Vortex Fluidic Device benefit from enhanced “on water” effects and copper jet feeds provide a convenient method of highly active catalyst delivery for flow chemistry.
Publisher: Wiley
Date: 04-2008
DOI: 10.1111/J.1742-4658.2008.06347.X
Abstract: Strategies for the chemical construction of synthetic proteins with precisely positioned post-translational modifications or their mimics offer a powerful method for dissecting the complexity of functional protein alteration and the associated complexity of proteomes.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8OB02130A
Abstract: A controlled-release fertiliser was prepared by the inverse vulcanisation of canola oil in the presence of nitrogen, phosphorous and potassium nutrients.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1SC05829K
Abstract: Micron to submicron size Coriolis and Faraday wave induced high shear topological flow regimes in 45° titled rapidly rotating tubes result in high inter-phase mass transfer of immiscible liquids and spontaneous demixing.
Publisher: American Chemical Society (ACS)
Date: 23-10-2009
DOI: 10.1021/JA907150M
Abstract: A phosphine-free palladium catalyst for aqueous Suzuki-Miyaura cross-coupling is presented. The catalyst is active enough to mediate hindered, ortho-substituted biaryl couplings but mild enough for use on peptides and proteins. The Suzuki-Miyaura couplings on protein substrates are the first to proceed in useful conversions. Notably, hydrophobic aryl and vinyl groups can be transferred to the protein surface without the aid of organic solvent since the aryl- and vinylboronic acids used in the coupling are water-soluble as borate salts. The convenience and activity of this catalyst prompts use in both general synthesis and bioconjugation.
Publisher: American Chemical Society (ACS)
Date: 23-09-2019
DOI: 10.26434/CHEMRXIV.9871898.V1
Abstract: High sulfur content polymers were prepared through the copolymerization of sustainable triglycerides and sulfur. The products of the so-called “inverse vulcanization” contain 50% sulfur by mass and were evaluated in the removal of inorganic and alkylmercury compounds from water. The structurally distinct triglycerides found in canola oil, castor oil, and rice bran oil were all examined as co-monomers in the inverse vulcanization reaction to determine how each influences the rate and capacity of mercury uptake. It was found that the high percentage of hydroxylated ricinoleic acid in castor oil improves both wetting and the rate of uptake of mercury(II) chloride into the polymer, in comparison to the polymers made from canola oil and rice bran oil. For the castor oil, the initial rate of uptake of mercury(II) chloride was more than three times the initial rate of uptake of the canola oil polymer, with a mercury removal efficiency exceeding 99.99%. The affinity of the castor oil polymer for HgCl2 was also excellent, with a distribution coefficient (Kd) on the order of 106 mL/g. In contrast, the polymer made from the inverse vulcanization of canola oil and sulfur had an initial rate of uptake more the twice the rate of the castor oil copolymer in experiments involving sorption of the mercury-based fungicide 2-methoxyethylmercury chloride (MEMC). In addition to kinetics, sorption isotherms were obtained for all polymer sorbents and fit to both Langmuir and Freundlich isotherm models. In terms of sustainability, this work advances the use renewable monomers such as triglycerides sourced from plants and inexpensive industrial byproducts such as sulfur to make affordable mercury-binding materials.
Publisher: American Chemical Society (ACS)
Date: 12-2021
DOI: 10.26434/CHEMRXIV-2021-JLL98
Abstract: There is growing interest in the bio-based production of lipids from algae. These lipids have a range of uses including nutritional supplements and precursors to biodiesel. Single-cell thraustochytrids are especially attractive in this regard in that they can produce over 50% of their weight as triglycerides. Furthermore, the distribution of saturated and unsaturated triglycerides can be modulated by changes in strain variation and modulation of fermentation conditions. Nonetheless, there remains a need for versatile downstream processing to enrich these so-called “single cell oils” into classes based on degree of unsaturation. In this study, we report a novel strategy for enriching saturated triglycerides produced in thraustochytrids. The method features direct reaction of elemental sulfur with the algae oil extract. The sulfur copolymerizes with % of the unsaturated triglycerides, providing a new route to a class of materials previously used in environmental remediation, Li-S battery cathodes, slow-release fertilisers, and insulation. The unreacted oil is enriched in saturated triglycerides, which can be isolated by extraction for potential use in biodiesel production. In this way, a single batch of sustainably produced algae oil can be converted into multiple useful products in a single step.
Publisher: American Chemical Society (ACS)
Date: 18-08-2007
DOI: 10.1021/OL701733U
Abstract: Two concise, high-yielding syntheses of enantioenriched (-)-kainic acid are presented. Both routes feature a Pd-catalyzed Zn-ene cyclization that proceeds with complete diastereoselectivity. The key step can be carried out on a multigram scale, and the overall yields are among the highest to date for this marine alkaloid.
Publisher: American Chemical Society (ACS)
Date: 03-06-2019
Publisher: American Association for the Advancement of Science (AAAS)
Date: 04-11-2016
Abstract: Chemically modifying proteins after their translation can expand their structural and functional roles (see the Perspective by Hofmann and Bode). Two related methods describe how to exploit free radical chemistry to form carbon-carbon bonds between amino acid residues and a selected functional group. Wright et al. added a wide range of functional groups to proteins containing dehydroalanine precursors, with borohydride mediating the radical chemistry. Yang et al. employed a similar approach, using zinc in combination with copper ions. Together, these results will be useful for introducing functionalities and labels to a wide range of proteins. Science , this issue pp. 597 and 623 see also p. 553
Publisher: Wiley
Date: 03-03-2008
Publisher: Elsevier BV
Date: 03-2018
Publisher: American Chemical Society (ACS)
Date: 05-07-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2009
DOI: 10.1039/B908004J
Abstract: Multiple, complementary methods are reported for the chemical conversion of cysteine to S-allyl cysteine on protein surfaces, a useful transformation for the exploration of olefin metathesis on proteins.
Publisher: Wiley
Date: 12-09-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C0CC03420G
Abstract: Statistical correlation of mass spectrum peak broadening with product dispersity in protein conjugation reactions allows more detailed characterization of putative therapeutic conjugates.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7GC00014F
Abstract: Polysulfide polymers prepared from elemental sulfur have found increasing use in applications that benefit the environment.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7RA11999B
Abstract: A polymer prepared by co-polymerisation of sulfur and canola oil removed Fe 3+ from water. Microwave irradiation was convenient in promoting the polymerisation.
Publisher: American Thoracic Society
Date: 15-09-2022
Publisher: Wiley
Date: 24-05-2023
Abstract: With increasing use of infrared imaging in medical diagnostics, military and civilian surveillance, and navigation of autonomous vehicles, there is a need for low‐cost alternatives to traditional materials used in infrared optics such as germanium. Sulfur‐rich copolymers hold promise, as they are made from low‐cost feedstocks and have a high refractive index. In this report, cyclopentadiene is copolymerized with sulfur to provide a plastic with the highest long‐wave infrared transparency reported to date for this class of materials. Diverse lens architectures are accessible through melt casting or reactive injection molding. The featured copolymer is black, which enabled its use as an infrared‐transparent blind for protection of thermal imaging equipment and clandestine surveillance. These findings portend expanded use of sulfur copolymers in infrared optics.
Publisher: Wiley
Date: 20-10-2016
Publisher: Wiley
Date: 08-04-2009
Abstract: For a reaction to be generally useful for protein modification, it must be site-selective and efficient under conditions compatible with proteins: aqueous media, low to ambient temperature, and at or near neutral pH. To engineer a reaction that satisfies these conditions is not a simple task. Olefin metathesis is one of most useful reactions for carbon-carbon bond formation, but does it fit these requirements? This minireview is an account of the development of olefin metathesis for protein modification. Highlighted below are ex les of olefin metathesis in peptidic systems and in aqueous media that laid the groundwork for successful metathesis on protein substrates. Also discussed are the opportunities in protein engineering for the genetic introduction of amino acids suitable for metathesis and the related challenges in chemistry and biology.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4RA01543F
Publisher: American Chemical Society (ACS)
Date: 07-02-2019
DOI: 10.26434/CHEMRXIV.7685654.V1
Abstract: Powdered activated carbon (PAC) is an economical sorbent for removing micropollutants from water, but it generates hazardous dust that is flammable and a respiration hazard. Additionally, the fine particles of PAC can cake and block filters and membranes, complicating its use in continuous processes. In this study, we present a sulfur polymer support for PAC that overcomes these problems. The blend of the sulfur polymer and PAC generates low dust and it does not block filters. The utility of the sorbent is demonstrated in the remediation of water contaminated with perfluorinated alkyl substances (PFASs)—persistent micropollutants that currently threaten water safety worldwide. Fundamental discoveries of PFAS self-assembly are reported, as well as testing on field s les.
Publisher: American Chemical Society (ACS)
Date: 05-04-2019
DOI: 10.26434/CHEMRXIV.7685654.V2
Abstract: Powdered activated carbon (PAC) is an economical sorbent for removing micropollutants from water, but it generates hazardous dust that is flammable and a respiration hazard. Additionally, the fine particles of PAC can cake and block filters and membranes, complicating its use in continuous processes. In this study, we present a sulfur polymer support for PAC that overcomes these problems. The blend of the sulfur polymer and PAC generates low dust and it does not block filters. The utility of the sorbent is demonstrated in the remediation of water contaminated with perfluorinated alkyl substances (PFASs)—persistent micropollutants that currently threaten water safety worldwide. Fundamental discoveries of PFAS self-assembly are reported, as well as testing on field s les.
Publisher: American Chemical Society (ACS)
Date: 08-05-2019
DOI: 10.26434/CHEMRXIV.7685654.V3
Abstract: Powdered activated carbon (PAC) is an economical sorbent for removing micropollutants from water, but it generates hazardous dust that is flammable and a respiration hazard. Additionally, the fine particles of PAC can cake and block filters and membranes, complicating its use in continuous processes. In this study, we present a sulfur polymer support for PAC that overcomes these problems. The blend of the sulfur polymer and PAC generates low dust and it does not block filters. The utility of the sorbent is demonstrated in the remediation of water contaminated with perfluorinated alkyl substances (PFASs)—persistent micropollutants that currently threaten water safety worldwide. Fundamental discoveries of PFAS self-assembly are reported, as well as testing on field s les.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CC07932A
Abstract: Allyl sulphides provoke rapid olefin metathesis when matched with an appropriate catalyst. In relay metathesis, allyl sulphides can serve as traceless promoters that facilitate the synthesis of non-sulphide targets.
Publisher: Cambridge University Press (CUP)
Date: 19-10-2021
DOI: 10.33774/CHEMRXIV-2021-N91H4
Abstract: The reaction between sulfur and dicyclopentadiene was optimised to form a shelf stable and soluble low molecular weight oligomer. After a simple curing process at 140 °C the material was rendered insoluble and resistant to acids and solvents. Taking advantage of the soluble oligomer, a metal surface was coated with the dissolved material which was then cured to show that a copolymer layer can act as a corrosion resistant material. Further, silica gel was coated with the soluble oligomer to test mercury removal applications. Even after curing, the polymer coated silica was an effective mercury sorbent. Additionally, the sorbent was also used to remove mercury form a diesel and water mixture indicating that mercury removal from a mixture of organic and aqueous substances is possible with this system.
Publisher: Wiley
Date: 31-03-2011
Publisher: American Chemical Society (ACS)
Date: 19-01-2022
Publisher: Wiley
Date: 18-04-2018
Publisher: American Chemical Society (ACS)
Date: 22-12-2020
DOI: 10.26434/CHEMRXIV.13464842.V1
Abstract: An insulating composite was made from the sustainable building blocks wool, sulfur, and canola oil. In the first stage of the synthesis, inverse vulcanization was used to make a polysulfide polymer from the canola oil triglyceride and sulfur. This polymerization benefits from complete atom economy. In the second stage, the powdered polymer is mixed with wool, coating the fibers through electrostatic attraction. The polymer and wool mixture is then compressed with mild heating to provoke S-S metathesis in the polymer, which locks the wool in the polymer matrix. The wool fibers impart tensile strength, insulating properties, and flame resistance to the composite. All building blocks are sustainable or derived from waste and the composite is a promising lead on next-generation insulation for energy conservation.
Publisher: Wiley
Date: 30-08-2017
Publisher: Wiley
Date: 17-12-2013
DOI: 10.1111/CBDD.12007
Publisher: Wiley
Date: 28-04-2009
Abstract: Chemical modification of proteins is a rapidly expanding area in chemical biology. Selective installation of biochemical probes has led to a better understanding of natural protein modification and macromolecular function. In other cases such chemical alterations have changed the protein function entirely. Additionally, tethering therapeutic cargo to proteins has proven invaluable in c aigns against disease. For controlled, selective access to such modified proteins, a unique chemical handle is required. Cysteine, with its unique reactivity, has long been used for such modifications. Cysteine has enjoyed widespread use in selective protein modification, yet new applications and even new reactions continue to emerge. This Focus Review highlights the enduring utility of cysteine in protein modification with special focus on recent innovations in chemistry and biology associated with such modifications.
Publisher: American Chemical Society (ACS)
Date: 06-07-2023
DOI: 10.26434/CHEMRXIV-2023-ZMBCN
Abstract: The principles of Green Chemistry and Engineering were formalised more than 20 years ago to guide us toward a safe and sustainable future. This framework is as important as ever in the development of chemical technologies that support human well-being while addressing the complex challenges we face in sustainability. This perspective is a reflection on the duty of chemists and engineers to integrate these principles into their practice, and how doing so can help confront erse problems such as climate change, sustainable food production, pollution control, renewable construction materials, and green energy production and storage.
Publisher: American Chemical Society (ACS)
Date: 16-07-2019
DOI: 10.26434/CHEMRXIV.8874077.V1
Abstract: Detection of cysteine sulfenic acid in live cells is critical in advancing our understanding of cysteine redox chemistry and its biological function. Accordingly, there is a need to develop sulfenic acid-specific chemical probes with distinct reaction mechanisms to facilitate proteome-wide detection of this important posttranslational modification. Herein, we report the first whole-cell proteomics analysis using a norbornene probe to detect cysteine sulfenic acid in live HeLa cells. Comparison of the enriched proteins to those identified using dimedone and other C -nucleophilic probes revealed a complementary reactivity profile. Remarkably, 148 new members of the sulfenome were identified. These discoveries highlight how subtle differences in chemical reactivity of both the probes and cysteine residues influence detection. Overall, this study expands our understanding of protein oxidation at cysteine and reveals new proteins to consider for future studies of cysteine oxidation, redox regulation and signaling, and the biochemistry of oxidative stress.
Publisher: American Chemical Society (ACS)
Date: 29-11-2018
DOI: 10.26434/CHEMRXIV.7396958.V1
Abstract: Norbornene derivatives were validated as probes for cysteine sulfenic acid on proteins and in live cells. Trapping sulfenic acids with norbornene probes is highly selective and revealed a different reactivity profile than the traditional dimedone reagent. The norbornene probe also revealed a superior chemoselectivity when compared to a commonly used dimedone probe. Together, these results advance the study of cysteine oxidation in biological systems.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1CC01555A
Abstract: A polymer made from sulfur and canola oil can be used as an oil spill sorbent and then repurposed into a sulfur-rich graphitic carbon for mercury removal from water.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3GC00785E
Abstract: TEMPO-functionalized surfactants are developed for the electrocatalytic oxidation of fatty alcohols to corresponding carbonyl compounds in water with up to 93% total conversion.
Publisher: Elsevier BV
Date: 12-2010
DOI: 10.1016/J.CBPA.2010.10.007
Abstract: The ability to alter protein structure by site-directed mutagenesis has revolutionized biochemical research. Controlled mutations at the DNA level, before protein translation, are now routine. These techniques allow specific, high fidelity interconversion largely between 20 natural, proteinogenic amino acids. Nonetheless, there is a need to incorporate other amino acids, both natural and unnatural, that are not accessible using standard site-directed mutagenesis and expression systems. Post-translational chemistry offers access to these side chains. Nearly half a century ago, the idea of a 'chemical mutation' was proposed and the interconversion between amino acid side chains was demonstrated on select proteins. In these isolated ex les, a powerful proof-of-concept was demonstrated. Here, we revive the idea of chemical mutagenesis and discuss the prospect of its general application in protein science. In particular, we consider amino acids that are chemical precursors to a functional set of other side chains. Among these, dehydroalanine has much potential. There are multiple methods available for dehydroalanine incorporation into proteins and this residue is an acceptor for a variety of nucleophiles. When used in conjunction with standard genetic techniques, chemical mutagenesis may allow access to natural, modified, and unnatural amino residues on translated, folded proteins.
Publisher: Wiley
Date: 24-01-2020
Abstract: Rapid detection of cysteine oxidation in living cells is critical in advancing our understanding of responses to reactive oxygen species (ROS) and oxidative stress. Accordingly, there is a need to develop chemical probes that facilitate proteome-wide detection of cysteine's many oxidation states. Herein, we report the first whole-cell proteomics analysis using a norbornene probe to detect the initial product of cysteine oxidation: cysteine sulfenic acid. The oxidised proteins identified in the HeLa cell model represent the first targets of the ROS hydrogen peroxide. The panel of protein hits provides new and important information about the targets of oxidative stress, including 148 new protein members of the sulfenome. These findings provide new leads for the study and understanding of redox signalling and diseases associated with oxidative stress.
Publisher: American Chemical Society (ACS)
Date: 17-02-2014
DOI: 10.1021/JO402799T
Abstract: The Suzuki-Miyaura cross-coupling reaction is a foundation stone of modern organic synthesis, as evidenced by its widespread use in the preparation of pharmaceuticals, agrochemicals, polymers, and other functional materials. With the prevalence of this venerable reaction in industrial synthesis, it is prudent to ensure its application adheres to the tenets of green chemistry. The introduction of cross-coupling catalysts that are active in sustainable solvents is therefore an important endeavor. In this report, a melamine-palladium complex is introduced as a versatile catalyst for the Suzuki-Miyaura cross-coupling reaction. This catalyst is soluble and active in both water and the renewable organic solvent ethyl lactate. The melamine-palladium catalyst can also be cross-linked by reaction with formaldehyde to generate an insoluble polymeric catalyst that can be recovered after the cross-coupling. The melamine-palladium system is inexpensive, easy to handle, bench-stable, and effective in catalysis in the presence of a variety of impurities (high cross-coupling yields were obtained in reactions run in unfiltered river water to illustrate this final point). Additionally, investigations reported herein revealed an intriguing relationship between catalytic efficiency and the base employed in the cross-coupling reaction. Implications for the mechanism of transmetalation in aqueous Suzuki-Miyaura cross-coupling reaction are discussed.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2PY00903J
Abstract: A magnetic responsive composite was made from a sulfur-rich polymer and iron nanoparticles. Diverse applications in mercury remediation, microwave curing, and magnetic responsive actuators were demonstrated.
Publisher: American Chemical Society (ACS)
Date: 20-03-2019
DOI: 10.1021/ACSCHEMBIO.8B01104
Abstract: Norbornene derivatives were validated as probes for cysteine sulfenic acid on proteins and in live cells. Trapping sulfenic acids with norbornene probes is highly selective and revealed a different reactivity profile than the traditional dimedone reagent. The norbornene probe also revealed a superior chemoselectivity when compared to a commonly used dimedone probe. Together, these results advance the study of cysteine oxidation in biological systems.
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C0SC00265H
Publisher: Springer Science and Business Media LLC
Date: 20-05-2019
DOI: 10.1007/S41061-019-0242-7
Abstract: Elemental sulfur is an abundant and inexpensive chemical feedstock, yet it is underused as a starting material in chemical synthesis. Recently, a process coined inverse vulcanization was introduced in which elemental sulfur is converted into polymers by ring-opening polymerization, followed by cross-linking with an unsaturated organic molecule such as a polyene. The resulting materials have high sulfur content (typically 50-90% sulfur by mass) and display a range of interesting properties such as dynamic S-S bonds, redox activity, high refractive indices, mid-wave IR transparency, and heavy metal affinity. These properties have led to a swell of applications of these polymers in repairable materials, energy generation and storage, optical devices, and environmental remediation. This article will discuss the synthesis of polymers by inverse vulcanization and review case studies on their erse applications. An outlook is also presented to discuss future opportunities and challenges for further advancement of polymers made by inverse vulcanization.
Publisher: Wiley
Date: 19-06-2015
Abstract: Thin film flow chemistry using a vortex fluidic device (VFD) is effective in the scalable acylation of amines under shear, with the yields of the amides dramatically enhanced relative to traditional batch techniques. The optimized monophasic flow conditions are effective in ≤80 seconds at room temperature, enabling access to structurally erse amides, functionalized amino acids and substituted ureas on multigram scales. Amide synthesis under flow was also extended to a total synthesis of local anesthetic lidocaine, with sequential reactions carried out in two serially linked VFD units. The synthesis could also be executed in a single VFD, in which the tandem reactions involve reagent delivery at different positions along the rapidly rotating tube with in situ solvent replacement, as a molecular assembly line process. This further highlights the versatility of the VFD in organic synthesis, as does the finding of a remarkably efficient debenzylation of p-methoxybenzyl amines.
Publisher: CSIRO Publishing
Date: 2015
DOI: 10.1071/CH15311
Abstract: Allyl sulfides have gained traction in recent years as promoters for olefin metathesis. The high reactivity of allyl sulfides in olefin metathesis is remarkable, given that many sulfur-containing substrates are incompatible with ruthenium-based olefin metathesis catalysts. In stark contrast, allyl sulfides actually enhance the rate of metathesis in comparison with other alkenes, when matched with a suitable catalyst. This review examines how the high reactivity of allyl sulfides in olefin metathesis has been harnessed in erse areas of synthesis. In the cases examined, allyl sulfides have been explicitly incorporated into substrates to promote olefin metathesis. Recent insights into catalyst considerations, applications in chemical and biochemical synthesis, and future opportunities are discussed.
Publisher: American Chemical Society (ACS)
Date: 28-03-2023
DOI: 10.26434/CHEMRXIV-2023-9NV60
Abstract: With increasing interest in high sulfur content polymers, there is a need to develop new methods for their synthesis that feature better safety and control of structure. In this report, electrochemically-initiated ring-opening polymerization of norbornene-based cyclic trisulfide monomers delivered well-defined, linear poly(trisulfides), which were solution processable. Electrochemistry provided a controlled initiation step that obviates the need for hazardous chemical initiators. The high temperatures required for inverse vulcanization are also avoided resulting in an improved safety profile. Density functional theory calculations revealed a reversible ‘self-correcting’ mechanism that ensures trisulfide linkages between monomer units. This control over sulfur rank is a new benchmark for high sulfur content polymers and creates opportunities to better understand the effects of sulfur rank on polymer properties. Thermogravimetric analysis coupled with mass spectrometry revealed the ability to recycle the polymer to the cyclic trisulfide monomer by thermal depolymerization. The featured poly(trisulfide) is an effective gold sorbent, with potential applications in mining and electronic waste recycling. A water-soluble poly(trisulfide) containing a carboxylic acid group was also produced and found to be effective in the binding and recovery of copper from aqueous media.
Publisher: Wiley
Date: 11-05-2018
Publisher: Wiley
Date: 24-10-2023
Publisher: American Chemical Society (ACS)
Date: 21-01-2022
DOI: 10.26434/CHEMRXIV-2022-SS450
Abstract: A polymer made from sulfur and limonene was used to coat silica gel and then evaluated as a mercury sorbent. A kinetic model of mercury uptake was established for a range of pH values and concentrations of sodium chloride. Mercury uptake was generally rapid from pH = 3 to pH = 11. At neutral pH, the sorbent (500 mg with a 10:1 ratio of silica to polymer) could remove 90% of mercury within one minute from a 100 mL solution 5 ppm in HgCl2 and 99% over 5 minutes. It was found that sodium chloride, at concentrations comparable to seawater, dramatically reduced mercury uptake rates and capacity. It was also found that the spent sorbent was stable in acidic and neutral media, but degraded at pH 11 which led to mercury leaching. These results help define the conditions under which the sorbent could be used, which is an important advance for using this material in remediation processes.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1NA00195G
Abstract: A rapidly rotating tube in the vortex fluidic device imparts submicron topological mass transport regimes, as moulded through crystallisation, polymerisation, and ‘molecular drilling’.
Publisher: Wiley
Date: 24-03-2010
Publisher: American Chemical Society (ACS)
Date: 20-12-2018
Publisher: American Chemical Society (ACS)
Date: 13-11-2017
Publisher: American Chemical Society (ACS)
Date: 25-10-2013
DOI: 10.1021/ED4002333
Publisher: Royal Society of Chemistry (RSC)
Date: 2008
DOI: 10.1039/B802199F
Abstract: A direct thionation procedure allows conversion of allylic alcohols into the corresponding thiols, the products of which are immediately compatible with one-pot site-selective selenenyl sulfide mediated protein conjugation.
Publisher: Wiley
Date: 05-02-2018
Publisher: Wiley
Date: 03-03-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3PY90102E
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7CS00607A
Abstract: Cysteine residues in proteins are subject to erse redox chemistry. Oxidation of cysteine to S-nitrosocysteine, cysteine sulfenic and sulfinic acids, disulfides and persulfides are a few prominent ex les of these oxidative post-translational modifications. In living organisms, these modifications often play key roles in cell signalling and protein function, but a full account of this biochemistry is far from complete. It is therefore an important goal in chemical biology to identify what proteins are subjected to these modifications and understand their physiological function. This review provides an overview of these modifications, how they can be detected and quantified using chemical probes, and how this information provides insight into their role in biology. This survey also highlights future opportunities in the study of cysteine redox chemistry, the challenges that await chemists and biologists in this area of study, and how meeting such challenges might reveal valuable information for biomedical science.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4OB02479F
Abstract: Halides are inhibitors of the copper-catalysed azide–alkyne cycloaddition. Case studies in this inhibition are presented, along with experimental measures useful in accommodating halides in this widely used reaction.
Publisher: Wiley
Date: 28-02-2023
Abstract: Heavy metal exposure has an enormous burden on human health. Current metal removal technologies require substantial improvements in relation to their efficiency and environmental impact if this issue is to be addressed. Over the last decade, several new types of sulfur‐rich sorbents have been investigated. These polymers typically have high removal efficiencies for toxic metals such as mercury and are often made using sustainable and low‐cost reagents. This review surveys polymers made by inverse vulcanization that have been tested for metal capture. Focus is put on environmental impact, feedstock for sorbent synthesis, selectivity towards metal removal, toxicity studies, and the reusability of the polymers. Furthermore, this review discusses current limitations and the potential opportunities to use different comonomers for improved metal capture.
Location: United Kingdom of Great Britain and Northern Ireland
Start Date: 2015
End Date: 2017
Funder: Australian Research Council
View Funded ActivityStart Date: 07-2021
End Date: 03-2024
Amount: $558,984.00
Funder: Australian Research Council
View Funded ActivityStart Date: 02-2020
End Date: 02-2023
Amount: $410,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 10-2022
End Date: 10-2026
Amount: $1,039,924.00
Funder: Australian Research Council
View Funded ActivityStart Date: 07-2021
End Date: 06-2024
Amount: $659,669.00
Funder: Australian Research Council
View Funded ActivityStart Date: 03-2017
End Date: 02-2020
Amount: $575,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 01-2015
End Date: 12-2017
Amount: $372,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2023
End Date: 12-2025
Amount: $405,186.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2021
End Date: 07-2023
Amount: $1,240,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2023
End Date: 04-2024
Amount: $620,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2019
End Date: 12-2020
Amount: $380,000.00
Funder: Australian Research Council
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