ORCID Profile
0000-0002-6142-3854
Current Organisation
Deakin University
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Transition Metal Chemistry | Inorganic Chemistry | Electroanalytical Chemistry
Publisher: American Chemical Society (ACS)
Date: 16-09-2020
Publisher: Wiley
Date: 11-08-2015
Abstract: To take advantage of the luminescent properties of d(6) transition metal complexes to label proteins, versatile bifunctional ligands were prepared. Ligands that contain a 1,2,3-triazole heterocycle were synthesised using Cu(I) catalysed azide-alkyne cycloaddition "click" chemistry and were used to form phosphorescent Ir(III) and Ru(II) complexes. Their emission properties were readily tuned, by changing either the metal ion or the co-ligands. The complexes were tethered to the metalloprotein transferrin using several conjugation strategies. The Ir(III)/Ru(II)-protein conjugates could be visualised in cancer cells using live cell imaging for extended periods without significant photobleaching. These versatile phosphorescent protein-labelling agents could be widely applied to other proteins and biomolecules and are useful alternatives to conventional organic fluorophores for several applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6AN00141F
Abstract: The first highly water soluble, blue-luminescent iridium( iii ) complex for chemiluminescence detection is presented.
Publisher: Wiley
Date: 11-12-2014
DOI: 10.1002/JLCR.3169
Abstract: New 1,4-substituted pyridyl-1,2,3-triazole ligands with pendent phenyl isothiocyanate functional groups linked to the heterocycle through a short methylene or longer polyethylene glycol spacers were prepared and conjugated to a peptide containing the arginine-glycine-aspartic acid peptide motif. Rhenium and technetium carbonyl complexes, [M(CO)3 L(x) (py)](+) (where M = Re(I) or (99m) Tc(I) L(x) = 1,4-substituted pyridyl-1,2,3-triazole ligands and py = pyridine) were prepared. One rhenium complex has been characterized by X-ray crystallography, and the luminescent properties of [M(CO)3 L(x) (py)](+) are reported.
Publisher: American Chemical Society (ACS)
Date: 13-01-2022
DOI: 10.1021/JACS.1C12059
Abstract: High-throughput synthesis and screening methods were used to measure the photochemical activity of 1440 distinct heteroleptic [Ir(C^N)
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4SC02697G
Abstract: The emissions of the mixed annihilation ECL of metal complexes can be effectively predicted by estimations of reaction exergonicity.
Publisher: Wiley
Date: 11-05-2015
Abstract: A unique two-step modular system for site-specific antibody modification and conjugation is reported. The first step of this approach uses enzymatic bioconjugation with the transpeptidase Sortase A for incorporation of strained cyclooctyne functional groups. The second step of this modular approach involves the azide-alkyne cycloaddition click reaction. The versatility of the two-step approach has been exemplified by the selective incorporation of fluorescent dyes and a positron-emitting copper-64 radiotracer for fluorescence and positron-emission tomography imaging of activated platelets, platelet aggregates, and thrombi, respectively. This flexible and versatile approach could be readily adapted to incorporate a large array of tailor-made functional groups using reliable click chemistry whilst preserving the activity of the antibody or other sensitive biological macromolecules.
Publisher: Wiley
Date: 18-08-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9SC05722F
Abstract: Visible light irradiation of 8-aminoquinoline Pd( ii ) complexes initiates photoinduced electron transfer with alkyl halides, affording C–H halogenation over C–C bond adducts. A method for inert C(sp 3 )–H bond halogenation (Br, Cl and I) is reported.
Publisher: American Chemical Society (ACS)
Date: 23-09-2019
DOI: 10.1021/JACS.9B07370
Abstract: We report the discovery of a tandem catalytic process to reduce energy demanding substrates, using the [Ir(ppy)
Publisher: Wiley
Date: 18-08-2020
Publisher: Wiley
Date: 08-05-2023
Abstract: We report a new composite material consisting of silver nanoparticles decorated with three‐dimensional molecular organic cages based on light‐absorbing porphyrins. The porphyrin cages serve to both stabilize the particles and allow diffusion and trapping of small molecules close to the metallic surface. Combining these two photoactive components results in a Fano‐resonant interaction between the porphyrin Soret band and the nanoparticle‐localised surface‐plasmon resonance. Time‐resolved spectroscopy revealed the silver nanoparticles transfer up to 37 % of their excited‐state energy to the stabilising layer of porphyrin cages. These unusual photophysics cause a 2‐fold current increase in photoelectrochemical water‐splitting measurements. The composite structure provides a compelling proof of concept for advanced photosensitiser systems with intrinsic porosity for photocatalytic and sensing applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2DT01491B
Abstract: Light is a critical reagent in photochemical synthesis but rarely considered beyond on or off controls. This Frontier article highlights recent ex les where photon delivery is controlled, affording unique reactivity.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8OB00238J
Abstract: A method for the light-driven synthesis of aryl and vinyl alkyl thioethers from a range of C(sp 2 )–I bonds is reported.
Publisher: American Chemical Society (ACS)
Date: 03-03-2016
DOI: 10.1021/ACS.INORGCHEM.5B02607
Abstract: A series of cyclometalated iridium(III) complexes with either 4-(2-pyridyl)-1,2,3-triazole or 1-(2-picolyl)-1,2,3-triazole ancillary ligands to give complexes with either 5- or 6-membered chelate rings were synthesized and characterized by a combination of X-ray crystallography, electron spin ionization-high-resolution mass spectroscopy (ESI-HRMS), and nuclear magnetic resonance (NMR) spectroscopy. The electronic properties of the complexes were probed using absorption and emission spectroscopy, as well as cyclic voltammetry. The relative stability of the complexes formed from each ligand class was measured, and their excited-state properties were compared. The emissive properties are, with the exception of complexes that contain a nitroaromatic substituent, insensitive to functionalization of the ancillary pyridyl-1,2,3-triazole ligand but tuning of the emission maxima was possible by modification of the cyclometalating ligands. It is possible to prepare a wide range of optimally substituted pyridyl-1,2,3-triazoles using copper Cu(I)-catalyzed azide alkyne cycloaddition, which is a commonly used "click" reaction, and this family of ligands represent an useful alternative to bipyridine ligands for the preparation of luminescent iridium(III) complexes.
Publisher: CSIRO Publishing
Date: 20-09-2023
DOI: 10.1071/CH23127
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9SC01391A
Abstract: A new strategy to create iridium( iii )-based ECL labels reveals limitations of conventional approaches.
Publisher: American Chemical Society (ACS)
Date: 30-04-2020
DOI: 10.26434/CHEMRXIV.12220109.V1
Abstract: We report a new visible light-mediated carbonylative amidation of aryl, heteroaryl and alkyl halides. A tandem catalytic cycle of [Ir(ppy) 2 (dtb-bpy)] + generates a potent iridium photoreductant via a second catalytic cycle in the presence of DIPEA which productively engages aryl bromides, iodides and even chlorides as well as primary, secondary and tertiary alkyl iodides. The versatility of the in-situ generated catalyst is illustrated by compatibility with aliphatic and aromatic amines, high functional group tolerance and the late-stage amidation of complex natural products.
Publisher: American Chemical Society (ACS)
Date: 10-07-2018
Publisher: American Chemical Society (ACS)
Date: 07-01-2021
DOI: 10.1021/JACS.0C12290
Publisher: Elsevier BV
Date: 09-2015
Publisher: Wiley
Date: 22-06-2017
Abstract: Modification of the local density of optical states using metallic nanostructures leads to enhancement in the number of emitted quanta and photocatalytic turnover of luminescent materials. In this work, the fabrication of a metamaterial is presented that consists of a nanowire separated from a metallic mirror by a polymer thin film doped with a luminescent organometallic iridium(III) complex. The large spin-orbit coupling of the heavy metal atom results in an excited state with significant magnetic-dipole character. The nanostructured architecture supports two distinct optical modes and their assignment achieved with the assistance of numerical simulations. The simulations show that one mode is characterized by strong confinement of the electric field and the other by strong confinement of the magnetic field. These modes elicit drastic changes in the emitter's photophysical properties, including dominant nanocavity-derived modes observable in the emission spectra along with significant increases in emission intensity and the total decay rate. A combination of simulations and momentum-resolved spectroscopy helps explain the mechanism of the different interactions of each optical mode supported by the metamaterial with the excited state of the emitter.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7CC03147E
Abstract: An oligoethylene glycol-containing photocleavable lysine tag was developed to facilitate the efficient synthesis and purification of the Aβ 42 peptide.
Publisher: Wiley
Date: 03-09-2015
Abstract: Incorporating phenylpyridine- and triazolylpyridine-based ligands decorated with methylsulfonate or tetraethylene glycol (TEG) groups, a series of iridium(III) complexes has been created for green and blue electrogenerated chemiluminescence under analytically useful aqueous conditions, with tri-n-propylamine as a coreactant. The relative electrochemiluminescence (ECL) intensities of the complexes were dependent on the sensitivity of the photodetector over the wavelength range and the pulse time of the applied electrochemical potential. In terms of the integrated area of corrected ECL spectra, with a pulse time of 0.5 s, the intensities of the Ir(III) complexes were between 18 and 102 % that of [Ru(bpy)3 ](2+) (bpy=2,2'-bipyridine). However, when the intensities were measured with a typical bialkali photomultiplier tube, the signal of the most effective blue emitter, [Ir(df-ppy)2 (pt-TEG)](+) (df-ppy=2-(2,4-difluorophenyl)pyridine anion, pt-TEG=1-(2-(2-(2-(2-hydroxyethoxy)ethoxy)ethoxy)ethyl)-4-(2-pyridyl)-1,2,3-triazole), was over 1200 % that of the orange-red emitter [Ru(bpy)3 ](2+) . A combined experimental and theoretical investigation of the electrochemical and spectroscopic properties of the Ir(III) complexes indicated that the greater intensity from [Ir(df-ppy)2 (pt-TEG)](+) relative to those of the other Ir(III) complexes resulted from a combination of many factors, rather than being significantly favored in one area.
Publisher: Elsevier BV
Date: 11-2018
Publisher: American Chemical Society (ACS)
Date: 07-01-2021
Publisher: American Chemical Society (ACS)
Date: 22-01-2019
Publisher: American Chemical Society (ACS)
Date: 21-02-2023
Publisher: Wiley
Date: 08-05-2023
Abstract: We report a new composite material consisting of silver nanoparticles decorated with three‐dimensional molecular organic cages based on light‐absorbing porphyrins. The porphyrin cages serve to both stabilize the particles and allow diffusion and trapping of small molecules close to the metallic surface. Combining these two photoactive components results in a Fano‐resonant interaction between the porphyrin Soret band and the nanoparticle‐localised surface‐plasmon resonance. Time‐resolved spectroscopy revealed the silver nanoparticles transfer up to 37 % of their excited‐state energy to the stabilising layer of porphyrin cages. These unusual photophysics cause a 2‐fold current increase in photoelectrochemical water‐splitting measurements. The composite structure provides a compelling proof of concept for advanced photosensitiser systems with intrinsic porosity for photocatalytic and sensing applications.
Publisher: Elsevier BV
Date: 09-2019
Publisher: Wiley
Date: 03-03-2014
Abstract: Compared to tris(2-phenylpyridine)iridium(III) ([Ir(ppy)3 ]), iridium(III) complexes containing difluorophenylpyridine (df-ppy) and/or an ancillary triazolylpyridine ligand [3-phenyl-1,2,4-triazol-5-ylpyridinato (ptp) or 1-benzyl-1,2,3-triazol-4-ylpyridine (ptb)] exhibit considerable hypsochromic shifts (ca. 25-60 nm), due to the significant stabilising effect of these ligands on the HOMO energy, whilst having relatively little effect on the LUMO. Despite their lower photoluminescence quantum yields compared with [Ir(ppy)3 ] and [Ir(df-ppy)3 ], the iridium(III) complexes containing triazolylpyridine ligands gave greater electrogenerated chemiluminescence (ECL) intensities (using tri-n-propylamine (TPA) as a co-reactant), which can in part be ascribed to the more energetically favourable reactions of the oxidised complex (M(+) ) with both TPA and its neutral radical oxidation product. The calculated iridium(III) complex LUMO energies were shown to be a good predictor of the corresponding M(+) LUMO energies, and both HOMO and LUMO levels are related to ECL efficiency. The theoretical and experimental data together show that the best strategy for the design of efficient new blue-shifted electrochemiluminophores is to aim to stabilise the HOMO, while only moderately stabilising the LUMO, thereby increasing the energy gap but ensuring favourable thermodynamics and kinetics for the ECL reaction. Of the iridium(III) complexes examined, [Ir(df-ppy)2 (ptb)](+) was most attractive as a blue-emitter for ECL detection, featuring a large hypsochromic shift (λmax =454 and 484 nm), superior co-reactant ECL intensity than the archetypal homoleptic green and blue emitters: [Ir(ppy)3 ] and [Ir(df-ppy)3 ] (by over 16-fold and threefold, respectively), and greater solubility in polar solvents.
Publisher: American Chemical Society (ACS)
Date: 11-01-2022
Publisher: Wiley
Date: 03-03-2020
Publisher: American Chemical Society (ACS)
Date: 15-06-2022
DOI: 10.1021/JACS.2C02011
Abstract: Photoredox catalysts are primarily selected based on ground and excited state properties, but their activity is also intrinsically tied to the nature of their reduced (or oxidized) intermediates. Catalyst reactivity often necessitates an inherent instability, thus these intermediates represent a mechanistic turning point that affords either product formation or side-reactions. In this work, we explore the scope of a previously demonstrated side-reaction that partially saturates one pyridine ring of the ancillary ligand in heteroleptic iridium(III) complexes. Using high-throughput synthesis and screening under photochemical conditions, we identified different chemical pathways, ultimately governed by ligand composition. The ancillary ligand was the key factor that determined photochemical stability. Following photoinitiated electron transfer from a sacrificial tertiary amine, the reduced intermediate of complexes containing 1,10-phenanthroline derivatives exhibited long-term stability. In contrast, complexes containing 2,2'-bipyridines were highly susceptible to hydrogen atom transfer and ancillary ligand modification. Detailed characterization of selected complexes before and after transformation showed differing effects on the ground and excited state reduction potentials dependent on the nature of the cyclometalating ligands and excited states. The implications of catalyst stability and reactivity in chemical synthesis was demonstrated in a model photoredox reaction.
Publisher: Wiley
Date: 22-10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CP01737A
Abstract: The annihilation electrogenerated chemiluminescence of mixtures of Ir( iii ) complexes is eliminated by manipulating reduction potentials through subtle changes in ligand structure.
Publisher: CSIRO Publishing
Date: 17-05-2022
DOI: 10.1071/CH21334
Abstract: The teaching laboratory remains an important environment for developing undergraduate chemists, but the inherent ersity of inorganic chemistry results in less standardised undergraduate curricula than other sub-disciplines. This study surveys the content of advanced (third-year) inorganic chemistry across Australia and reviews experimental materials from 15 universities that offer inorganic laboratory programmes at this level. All institutions offer at least one traditional inorganic experiment, the most common being the preparation and acetylation of ferrocene, spectroscopy and magnetochemistry of nickel coordination compounds and palladium-catalysed cross-couplings. These inorganic classics are complemented by a breadth of non-traditional offerings that often align with institutional research strengths. Academic unit coordinators were also surveyed and their responses interpreted using ASELL (Advancing Science and Engineering through Laboratory Learning) tools. Advanced inorganic laboratory programmes were found to develop students’ practical and transferrable skills. Students generally receive guidance from teaching staff in all aspects of experimental work, including planning, development, analysis and communicating conclusions. Academic unit coordinators identified potential improvements that included ersifying student activities in the lab and how they are being assessed.
Publisher: American Chemical Society (ACS)
Date: 07-01-2019
Publisher: Informa UK Limited
Date: 15-07-2022
Publisher: American Chemical Society (ACS)
Date: 20-06-2014
DOI: 10.1021/IC5008999
Abstract: The synthesis and characterization of a silver complex of the tripodal triazole ligand, tris(benzyltriazolylmethyl)amine (TBTA, L(1)), that is used as promoter to enhance Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reactions is reported. X-ray analysis of the silver(I) complex with L(1) reveals a dinuclear cation, [Ag2(L(1))2](2+), that is essentially isostructural to the copper(I) analogue. While the [Ag2(L(1))2](BF4)2 complex provides catalysis for the azide-alkyne cycloaddition process, evidence is presented that this arises from trace copper contamination. The synthesis of silver(I), copper(II), and copper(I) complexes of a second tripodal ligand, tris(2-benzimidazolymethyl)amine (L(2)), which is used to enhance the rate of CuAAC reactions, is also reported. X-ray crystallography of the Cu(I) complex [Cu(I)3(L(2))2(CH3CN)2](BF4)3 offers structural insight into previous mechanistic speculation about the role of this ligand in the CuAAC reaction.
Publisher: American Chemical Society (ACS)
Date: 24-02-2021
Publisher: American Chemical Society (ACS)
Date: 26-09-2018
Publisher: American Chemical Society (ACS)
Date: 28-05-2020
Publisher: Optica Publishing Group
Date: 23-11-2020
Abstract: The optoelectronic properties of asymmetric metal nanostructures are of current interest for applications in photonics, sensing, and catalysis. Here, we break the symmetry of the localized surface plasmon resonance of gold nanorods by selective overgrowth of a single tip via a high-yield ( --> 80 % ) wet-chemical method. While optical spectroscopy exhibits a bathochromic shift of the nanoparticle plasmon resonance, cathodoluminescence and electron energy loss spectroscopy measurements reveal a breaking of the symmetry of the associated localized surface plasmon resonance mode, which results in the subwavelength concentration of electromagnetic energy. The simple, one-step postsynthetic modification allows control of nanoparticle structural parameters, and we demonstrate how the asymmetric energy redistribution leads to increases in the surface-enhanced Raman scattering of a model analyte attached to the surface of the nanostructures. The spatial localization of energy in these nanostructures may find applications in nanofocusing, nanoimaging, and light harvesting.
Start Date: 02-2022
End Date: 02-2025
Amount: $462,873.00
Funder: Australian Research Council
View Funded ActivityStart Date: 07-2021
End Date: 06-2024
Amount: $430,000.00
Funder: Australian Research Council
View Funded Activity