ORCID Profile
0000-0001-7672-9795
Current Organisation
University of New South Wales
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Structural Chemistry and Spectroscopy | Macromolecular and Materials Chemistry | Nanochemistry and Supramolecular Chemistry | Electrochemistry | Synthesis of Materials | Transition Metal Chemistry | Physical Chemistry (Incl. Structural)
Hydrogen Storage | Expanding Knowledge in the Chemical Sciences | Energy Storage (excl. Hydrogen) |
Publisher: Wiley
Date: 19-02-2020
Abstract: The resurgence of interest in the hydrogen economy could hinge on the distribution of hydrogen in a safe and efficient manner. Whilst great progress has been made with cryogenic hydrogen storage or liquefied ammonia, liquid organic hydrogen carriers (LOHCs) remain attractive due to their lack of need for cryogenic temperatures or high pressures, most commonly a cycle between methylcyclohexane and toluene. Oxidation of methylcyclohexane to release hydrogen will be more efficient if the equilibrium limitations can be removed by separating the mixture. This report describes a family of six ternary and quaternary multicomponent metal-organic frameworks (MOFs) that contain the three-dimensional cubane-1,4-dicarboxylate (cdc) ligand. Of these MOFs, the most promising is a quaternary MOF (CUB-30), comprising cdc, 4,4'-biphenyldicarboxylate (bpdc) and tritopic truxene linkers. Contrary to conventional wisdom that adsorptive interactions with larger, hydrocarbon guests are dominated by π-π interactions, here we report that contoured aliphatic pore environments can exhibit high selectivity and capacity for LOHC separations at low pressures. This is the first time, to the best of our knowledge, where selective adsorption for cyclohexane over benzene is witnessed, underlining the unique adsorptive behavior afforded by the unconventional cubane moiety.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9CC00206E
Abstract: A photoactive Co II /Ru II -based MOF with a channel aperture of ca. 21 Å is reported its gas sorption behavior is characteristic of mesoporous materials with CO 2 sorption selectivity over N 2 .
Publisher: Wiley
Date: 09-07-2021
Abstract: Im Wesentlichen hat die retikuläre Chemie die Präzision und Expertise der organischen und anorganischen Synthese auf den festen Zustand übertragen. Während die anfängliche Aufregung über Metall‐organische Gerüstverbindungen (MOFs) und kovalente organische Gerüstverbindungen (COFs) zweifellos durch ihre beispiellose Porosität und Oberfläche befeuert wurde, war die tiefgreifendste wissenschaftliche Innovation des Feldes die Ausarbeitung von Designstrategien für die Synthese von erweiterten kristallinen Festkörpern durch starke gerichtete Bindungen. In diesem Aufsatz beleuchten wir die verschiedenen Klassen von retikulären Materialien, die entwickelt worden sind, wie solche Gerüstverbindungen funktionalisiert werden können und wie Komplexität in ihr Grundgerüst eingeführt werden kann. Schließlich zeigen wir, wie die strukturelle Kontrolle über diese Materialien von der molekularen Skala über ihre Kristallmorphologie und Form auf der Nanoskala bis hin zu ihrer Gestaltung auf der Bulk‐Skala erweitert wird.
Publisher: American Chemical Society (ACS)
Date: 18-02-2019
DOI: 10.1021/JACS.8B13639
Abstract: One prominent aspect of metal organic frameworks (MOFs) is the ability to tune the size, shape, and chemical characteristics of their pores. MOF-5, with its open cubic connectivity of Zn
Publisher: CSIRO Publishing
Date: 2014
DOI: 10.1071/CH14355
Abstract: A range of ethylxanthate (EtXn) salts, containing either protic or aprotic cations (guanidinium (1), methylammonium (2), dimethylammonium (3), trimethylammonium (4), tetramethylammonium (5), tetraethylammonium (6), and tetrapropylammonium (7)), have been synthesised and structurally characterised. The cations in these compounds differ in their degree of hydrogen-bonding ability, i.e. the number of donor groups, with significant structural consequences. Compounds 1–4 contain cations that are able to form N–H···S hydrogen bonds, with six, three, two, and one donor groups in 1–4 respectively. The number of donor atoms affects greatly the dimensionality of the hydrogen-bonding networks in the solid state. The structure of 1 has a 3-D hydrogen-bonding network, 2 and 3 form 2-D sheets and 1-D chains respectively, whereas the lone NH donor group in 4 has strong hydrogen bonding only within a discrete cation–anion pair. The tetraalkylammonium salts 5–7 have no strong hydrogen bonding, with only C–H···S and C–H···O interactions possible. To determine unambiguously the presence of such interactions, single-crystal Laue neutron diffraction data were obtained for compound 5, providing a fully anisotropic model, which can be used to rationalise potential close interactions in the other structures. The neutron structure of 5 confirms the existence of C–H···S hydrogen bonds, with the H···S distance falling well within the sum of the van der Waals radii of the atoms. The close-packing in 5–7 is mediated solely through these weak interactions, with the size of the cations influencing the structures.
Publisher: American Chemical Society (ACS)
Date: 05-11-2021
Publisher: Elsevier BV
Date: 2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0TA11229A
Abstract: MOF crystal-glass composites (MOF CGCs) are materials with crystalline MOFs embedded within a MOF glass. Here we develop two novel MOF CGCs, and explore the gas uptake and guest-size limitations within these materials.
Publisher: Wiley
Date: 08-09-2014
Abstract: A series of soluble metal ethylxanthate compounds was synthesised as precursors for metal sulfide thin films to be deposited using solution‐based techniques. Initially, a range of air‐ and moisture‐stable organic ethylxanthate (EtXn) salts were synthesised (cation=Me 4 N ( 1 ), Et 4 N ( 2 ), Pr 4 N ( 3 ), Ph 4 P ( 4 ), guanidinium ( 5 ), NMeH 3 ( 6 ), NMe 2 H 2 ( 7 ), NMe 3 H ( 8 ), NH 4 ( 9 )). Thermogravimetric analysis (TGA) was used to examine their decomposition profiles, which in turn informed the decision of which counter cation was best suited for inclusion in the metal xanthate compounds. Periodic NMR spectroscopy studies and single‐crystal X‐ray diffraction (SXRD) were used to determine the role protic ammonium counter cations play in the detrimental conversion of xanthates to dithiocarbamate anions. The organic salts 1 and 4 were used to form the metal ethylxanthate compounds (Me 4 N)[M(EtXn) x ] ( x =3 for M=Cd ( 10 Cd ), Ni ( 10 Ni ), Zn ( 10 Zn ) x =4 for M=La ( 11 La )) and (Ph 4 P)[M(EtXn) 3 ] (M=Cd ( 12 Cd ), Ni ( 12 Ni ), Zn ( 12 Zn )). Solubility studies on these compounds were performed using a range of solvents to demonstrate the viability of using these compounds for solution‐based deposition methods for thin‐film formation. TGA of the metal xanthate compounds was used to examine their thermal‐decomposition profiles and the product resulting from thermolysis was found to be the respective metal sulfide. In addition, the coproducts of thermal decomposition were analysed by headspace gas‐chromatography mass spectrometry (HS GC–MS) to probe the decomposition mechanism of the precursors. In situ variable‐temperature synchrotron XRD studies on both bulk and thin‐film s les of 10 Cd and 12 Cd were used to examine metal sulfide crystalline phase formation. Decomposition of both precursors was found to give CdS in a hexagonal phase, with the addition of CdCl 2 found to aid in increasing the crystallite size during crystallisation.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1OB01545A
Abstract: The acridinone 1,9-bis(thio)urea scaffold was repurposed for application in anion transport by appending a variety of electron-withdrawing groups to the peripheral phenyl moieties. High levels of activity were achieved which facilitated strictly electroneutral transport.
Publisher: Wiley
Date: 03-05-2023
Abstract: Metal‐organic frameworks (MOFs) are a class of porous materials with high surface areas, which are acquiring rapid attention on an exponential basis. A significant characteristic of MOFs is their ability to act as adsorbents to selectively separate component mixtures of similar size, thereby addressing the technological need for an alternative approach to conventional distillation methods. Recently, MOFs comprising a 3‐Dimensional (3D) linker have shown outstanding capabilities for difficult separations compared to the parent 2‐Dimensional (2D) analogue. 3D‐linkers with a polycyclic core are underrepresented in the MOF database due to the widespread preferred use of 2D‐linkers and the misconceived high‐cost of 3D linkers. We summarize the recent research of 3D‐linker MOFs and highlight their beneficial employment for selective gas and hydrocarbon adsorption and separation. Furthermore, we outline forecasts in this area to create a platform for widespread adoption of 3D‐linkers in MOF synthesis.
Publisher: Elsevier BV
Date: 02-2022
DOI: 10.1016/J.BBAMEM.2021.183828
Abstract: Phenylthiosemicarbazones (PTSCs) are proton-coupled anion transporters with pH-switchable behaviour known to be regulated by an imine protonation equilibrium. Previously, chloride/nitrate exchange by PTSCs was found to be inactive at pH 7.2 due to locking of the thiourea anion binding site by an intramolecular hydrogen bond, and switched ON upon imine protonation at pH 4.5. The rate-determining process of the pH switch, however, was not examined. We here develop a new series of PTSCs and demonstrate their conformational behaviour by X-ray crystallographic analysis and pH-switchable anion transport properties by liposomal assays. We report the surprising finding that the protonated PTSCs are extremely selective for halides over oxyanions in membrane transport. Owing to the high chloride over nitrate selectivity, the pH-dependent chloride/nitrate exchange of PTSCs originates from the rate-limiting nitrate transport process being inhibited at neutral pH.
Publisher: CSIRO Publishing
Date: 17-01-2022
DOI: 10.1071/CH21208
Abstract: Lightweight metal–organic frameworks (MOFs) with large volume storage capabilities are highly sought after as solid adsorbents in gas storage applications. This is particularly important for hydrogen gas adsorbents and can be explored through constructing MOFs from magnesium, which is a light metal and can readily form lightweight frameworks. Recently, the use of bulky, 3D aliphatic linkers in MOF synthesis has resulted in materials with higher gas adsorption enthalpies at lower pressures. Here, we employ both aliphatic linkers and magnesium clusters to produce lightweight, aliphatic frameworks with potential use for gas adsorption applications. Two magnesium MOFs were synthesised, 3DL-MOF-2 and 3DL-MOF-3 (3DL = 3DLinker), and structurally investigated using single crystal X-ray diffraction. While these MOFs do not have any accessible void spaces and therefore cannot be used for gas adsorption, they create a platform for future magnesium aliphatic MOF research to form open frameworks.
Publisher: Wiley
Date: 09-07-2021
Abstract: At its core, reticular chemistry has translated the precision and expertise of organic and inorganic synthesis to the solid state. While initial excitement over metal–organic frameworks (MOFs) and covalent organic frameworks (COFs) was undoubtedly fueled by their unprecedented porosity and surface areas, the most profound scientific innovation of the field has been the elaboration of design strategies for the synthesis of extended crystalline solids through strong directional bonds. In this contribution we highlight the different classes of reticular materials that have been developed, how these frameworks can be functionalized, and how complexity can be introduced into their backbones. Finally, we show how the structural control over these materials is being extended from the molecular scale to their crystal morphology and shape on the nanoscale, all the way to their shaping on the bulk scale.
Publisher: Elsevier BV
Date: 03-2021
Publisher: Springer Science and Business Media LLC
Date: 26-11-2021
Publisher: Wiley
Date: 19-02-2020
Publisher: MDPI AG
Date: 06-11-2020
DOI: 10.3390/MOLECULES25215179
Abstract: Synthetic anion transporters that facilitate chloride transport are promising candidates for channelopathy treatments. However, most anion transporters exhibit an undesired side effect of facilitating proton transport via interacting with fatty acids present in the membrane. To address the limitation, we here report the use of a new tetrapodal scaffold to maximize the selective interaction with spherical chloride over binding the carboxylate headgroup of fatty acids. One of the new transporters demonstrated a high selectivity for chloride uniport over fatty acid-induced proton transport while being times more active in chloride uniport than strapped calixpyrroles that were previously the only class of compounds known to possess similar selectivity properties.
Publisher: Elsevier BV
Date: 06-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC03737J
Abstract: The first cadmium-based ionic liquids (ILs) have been developed, along with a family of cadmium dialkyldithiocarbamate salts, (cation)[Cd(R 2 dtc) 3 ], in the pursuit of single source molecular precursors that thermolyse to form cadmium sulfide.
Publisher: American Chemical Society (ACS)
Date: 29-07-2020
Publisher: Wiley
Date: 04-09-2014
Publisher: American Chemical Society (ACS)
Date: 20-10-2023
DOI: 10.1021/JACS.3C04641
Publisher: American Chemical Society (ACS)
Date: 24-06-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9DT00075E
Abstract: Top-down, synthetic approaches provide new pathways to functionalised hybrid polyoxometalates (POMs).
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA08449F
Abstract: Fe-BTC, a disordered metal–organic framework, exhibits clear discrimination of propene and propane compared to its crystalline counterpart MIL-100.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC05715K
Abstract: Mixed donor phenanthroline-carboxylate linkers were combined with Mn II or Zn II to form photoactive MOFs with large pore apertures.
Publisher: Elsevier BV
Date: 04-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CE00784G
Publisher: American Chemical Society (ACS)
Date: 10-03-2023
DOI: 10.1021/JACS.2C13715
Publisher: Wiley
Date: 03-05-2023
Abstract: Metal‐organic frameworks (MOFs) are a class of porous materials with high surface areas, which are acquiring rapid attention on an exponential basis. A significant characteristic of MOFs is their ability to act as adsorbents to selectively separate component mixtures of similar size, thereby addressing the technological need for an alternative approach to conventional distillation methods. Recently, MOFs comprising a 3‐Dimensional (3D) linker have shown outstanding capabilities for difficult separations compared to the parent 2‐Dimensional (2D) analogue. 3D‐linkers with a polycyclic core are underrepresented in the MOF database due to the widespread preferred use of 2D‐linkers and the misconceived high‐cost of 3D linkers. We summarize the recent research of 3D‐linker MOFs and highlight their beneficial employment for selective gas and hydrocarbon adsorption and separation. Furthermore, we outline forecasts in this area to create a platform for widespread adoption of 3D‐linkers in MOF synthesis.
Location: Australia
Start Date: 01-2023
End Date: 01-2026
Amount: $602,766.00
Funder: Australian Research Council
View Funded ActivityStart Date: 04-2023
End Date: 04-2023
Amount: $597,373.00
Funder: Australian Research Council
View Funded ActivityStart Date: 05-2021
End Date: 01-2025
Amount: $447,625.00
Funder: Australian Research Council
View Funded Activity