ORCID Profile
0000-0003-0215-5922
Current Organisation
University of Adelaide
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Macromolecular and Materials Chemistry | Synthesis of Materials | Transition Metal Chemistry | Nanochemistry and Supramolecular Chemistry | Separation Science | Chemical Characterisation of Materials
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CE01030J
Abstract: Metal–organic frameworks are highly crystalline porous materials which present emerging opportunities in biotechnology, catalysis, microelectronics and photonics.
Publisher: American Chemical Society (ACS)
Date: 21-07-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5DT05023E
Abstract: Mixed-ligand syntheses and post-synthetic metal exchange performed on the Mn 3 L 3 structure type results in site-specific manipulations to the framework structure.
Publisher: American Chemical Society (ACS)
Date: 22-10-2011
DOI: 10.1021/ED100001S
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C0SC00179A
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CE00746B
Abstract: Nanoscale structuralisation is demonstrated to influence the stability and catalytic properties of zeolitic imidazolate framework-8.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5TA05620A
Abstract: Size selective adsorption of alcohols and molecular recognition of methanol over water are observed in the heterostructured Zn 4 O(3,5-dialkylcarboxypyrazolate) 3 films.
Publisher: American Chemical Society (ACS)
Date: 13-03-2013
DOI: 10.1021/JA312115X
Abstract: Understanding the sorption kinetics of nanoporous systems is crucial for the development and design of novel porous materials for practical applications. Here, using a porous coordination polymer/quartz crystal microbalance (PCP/QCM) hybrid device, we investigate the desorption of various vapor molecules featuring different degrees of intermolecular (hydrogen bonding) or molecule-framework interactions. Our findings reveal that strong intermolecular interactions lead to the desorption process proceeding via an unprecedented metastable state, wherein the guest molecules are clustered within the pores, causing the desorption rate to be temporarily slowed. The results demonstrate the considerable impact of the chemical nature of an adsorbate on the kinetics of desorption, which is also expected to influence the efficiency of certain processes, such as desorption by gas purge.
Publisher: IEEE
Date: 02-2010
Publisher: American Chemical Society (ACS)
Date: 22-03-2016
DOI: 10.1021/ACS.INORGCHEM.6B00397
Abstract: The emergence of metal-organic frameworks (MOFs) as potential candidates to supplant existing adsorbent types in real-world applications has led to an explosive growth in the number of compounds available to researchers, as well as in the ersity of the metal salts and organic linkers from which they are derived. In this context, the use of carbonate-based precursors as metal sources is of interest due to their abundance in mineral deposits and their reaction chemistry with acids, resulting in just water and carbon dioxide as side products. Here, we have explored the use of calcium carbonate as a metal source and demonstrate its versatility as a precursor to several known frameworks, as well as a new flexible compound based on the 2,5-dihydroxybenzoquinone (H2dhbq) linker, Ca(dhbq)(H2O)2. Furthermore, inspired by the ubiquity and unique structures of biomineralized forms of calcium carbonate, we also present ex les of the preparation of superstructures of Ca-based MOFs via the coordination replication technique. In all, the results confirm the suitability of carbonate-based metal sources for the preparation of MOFs and further expand upon the growing scope of coordination replication as a convenient strategy for the preparation of structuralized materials.
Publisher: The Optical Society
Date: 05-2014
DOI: 10.1364/OE.22.011061
Publisher: Royal Society of Chemistry (RSC)
Date: 2008
DOI: 10.1039/B716189A
Abstract: The reactions of boron halides with free base porphyrins under conditions where partial hydrolysis of the boron halides can occur give diboron porphyrin complexes containing BOB moieties in which each boron is bonded to two porphyrin nitrogen atoms. BF(3).OEt(2) with H(2)(por) gives B(2)OF(2)(por) (por = tpp, ttp, tpClpp, oep) which has an asymmetric structure in which one boron lies in the porphyrin plane (B(ip)) while the other lies above it (B(oop)). BCl(3).MeCN with H(2)(por) gives B(2)O(2)(BCl(3))(2)(por) which contains a four-membered B(2)O(2) ring and is stable only in the presence of excess BCl(3). BBr(3) with Li(2)(tpClpp) gives the dicationic complex [B(2)O(tpClpp)](2+) as its [BBr(4)](-) salt, and is the first ex le of a boron porphyrin containing three-coordinate boron to be structurally characterised. B(2)O(2)(BCl(3))(2)(por) can be chromatographed on basic alumina to give the hydroxyboron complex B(2)O(OH)(2)(por), which is deduced from its NMR spectra and DFT calculations to have a structure analogous to B(2)OF(2)(por). The OH protons are shifted upfield to near delta -4 (B(oop)-OH) and -10 (B(ip)-OH) by the diamagnetic porphyrin ring current. The reaction of either B(2)O(2)(BCl(3))(2)(por) or B(2)O(OH)(2)(por) (por = ttp, tpClpp) with alcohols (ROH, R = Et, 4-C(6)H(4)CH(3)) gives B(2)O(OR)(2)(por), which can in turn be converted to B(2)O(OR)(OH)(por) by repeated chromatography. The reaction of PhBCl(2) with H(2)(por) (por = ttp, tpClpp) gives B(2)O(Ph)(OH)(por) which has been characterised by spectroscopy in concert with DFT calculations. It is a further ex le of the B(2)OF(2)(por) structural type, in which the phenyl group is coordinated to the out-of-plane boron and the OH group to the in-plane boron, as are its derivatives B(2)O(Ph)(X)(tpClpp) (X = F, OEt). Steric drivers for the facile hydrolysis of haloboron porphyrins relative to their dipyrromethene and expanded porphyrin counterparts are discussed.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C0CC03453C
Abstract: The hydrogen storage properties of Mg(2)(dobdc) (dobdc(4-) = 2,5-dioxido-1,4-benzenedicarboxylate), a metal-organic framework possessing hexagonal one-dimensional channels decorated with unsaturated Mg(2+) coordination sites, have been examined through low- and high-pressure adsorption experiments, infrared spectroscopy, and neutron scattering studies.
Publisher: American Chemical Society (ACS)
Date: 06-04-2015
DOI: 10.1021/JACS.5B00838
Abstract: Despite the large number of metal-organic frameworks that have been studied in the context of post-combustion carbon capture, adsorption equilibria of gas mixtures including CO2, N2, and H2O, which are the three biggest components of the flue gas emanating from a coal- or natural gas-fired power plant, have never been reported. Here, we disclose the design and validation of a high-throughput multicomponent adsorption instrument that can measure equilibrium adsorption isotherms for mixtures of gases at conditions that are representative of an actual flue gas from a power plant. This instrument is used to study 15 different metal-organic frameworks, zeolites, mesoporous silicas, and activated carbons representative of the broad range of solid adsorbents that have received attention for CO2 capture. While the multicomponent results presented in this work provide many interesting fundamental insights, only adsorbents functionalized with alkylamines are shown to have any significant CO2 capacity in the presence of N2 and H2O at equilibrium partial pressures similar to those expected in a carbon capture process. Most significantly, the amine-appended metal organic framework mmen-Mg2(dobpdc) (mmen = N,N'-dimethylethylenediamine, dobpdc (4-) = 4,4'-dioxido-3,3'-biphenyldicarboxylate) exhibits a record CO2 capacity of 4.2 ± 0.2 mmol/g (16 wt %) at 0.1 bar and 40 °C in the presence of a high partial pressure of H2O.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3TC32101K
Publisher: Wiley
Date: 27-06-2014
Abstract: We demonstrate a new approach to superhydrophobic porous coordination polymers by incorporating an anisotropic crystal morphology featuring a predominant surface that is highly corrugated and terminated by aromatic hydrocarbon moieties. The resulting low-energy surface provides particularly promising hydrophobic properties without the need for postsynthetic modifications or surface processing that would block the porosity of the framework. Consequently, hydrophobic organic molecules and water vapor are able to penetrate the surface and be densely accommodated within the pores, whereas bulk water is repelled as a result of the exterior surface corrugation derived from the aromatic surface groups. This study provides a new strategy for the design and development of superhydrophobic porous materials.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CC09694K
Abstract: Robust, hierarchically porous Cu 3 (btc) 2 (HKUST-1, btc 3− = benzene-1,3,5-tricalboxylate) monoliths have been synthesized by direct conversion of sol–gel-derived Cu(OH) 2 -based monoliths.
Publisher: Springer Science and Business Media LLC
Date: 15-08-2020
Publisher: Wiley
Date: 05-07-2010
Abstract: The reaction of CuCl 2 · 2H 2 O with three novel ditopic ligands, 2‐methyl‐1,4‐benzeneditetrazolate (MeBDT 2– ), 4,4′‐biphenylditetrazolate (BPDT 2– ), and 2,3,5,6‐tetrafluoro‐1,4‐benzeneditriazolate (TFBDTri 2– ), affords the metal–organic frameworks Cu(MeBDT)(dmf) ( 1 ), Cu(BPDT)(dmf) ( 2 ), and Cu(TFBDTri)(dmf) ( 3 ), respectively. These materials feature a common network topology in which octahedral Cu 2+ ions are bridged by azolate ligands and dmf molecules to form one‐dimensional chains. The in idual chains are connected by the organic bridging units to form diamond‐shaped channels, in which the solvent molecules project into the pores. The bridging dmf molecules in 1 are readily displaced by other coordinating solvent molecules, which leads to a change in the pore dimensions according to the steric bulk of the solvent. Interestingly, attempts to exchange the analogous solvent molecules in the expanded framework 2 induced no change in the pore size, revealing the rigidity of the framework. Meanwhile, 3 exhibits modest flexibility and an improved thermal stability consistent with its chemical functionality. The marked difference in flexibility highlights the considerable impact the organic linker can have on the dynamic framework properties.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1EE01720A
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5SC02034D
Abstract: Monolithic superstructures of two- and three-dimensional flexible frameworks are prepared via coordination replication from a copper hydroxide parent phase.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C2EE23337A
Publisher: American Chemical Society (ACS)
Date: 02-10-2009
DOI: 10.1021/JA9072707
Abstract: The first crystalline beryllium-based metal-organic framework has been synthesized and found to exhibit an exceptional surface area useful for hydrogen storage. Reaction of 1,3,5-benzenetribenzoic acid (H(3)BTB) and beryllium nitrate in a mixture of DMSO, DMF, and water at 130 degrees C for 10 days affords the solvated form of Be(12)(OH)(12)(1,3,5-benzenetribenzoate)(4) (1). Its highly porous framework structure consists of unprecedented saddle-shaped [Be(12)(OH)(12)](12+) rings connected through tritopic BTB(3-) ligands to generate a 3,12 net. Compound 1 exhibits a BET surface area of 4030 m(2)/g, the highest value yet reported for any main group metal-organic framework or covalent organic framework. At 77 K, the H(2) adsorption data for 1 indicate a fully reversible uptake of 1.6 wt % at 1 bar, with an initial isosteric heat of adsorption of -5.5 kJ/mol. At pressures up to 100 bar, the data show the compound to serve as an exceptional hydrogen storage material, reaching a total uptake of 9.2 wt % and 44 g/L at 77 K and of 2.3 wt % and 11 g/L at 298 K. It is expected that reaction conditions similar to those reported here may enable the synthesis of a broad new family of beryllium-based frameworks with extremely high surface areas.
Publisher: Wiley
Date: 23-09-2013
Publisher: American Chemical Society (ACS)
Date: 28-12-2011
DOI: 10.1021/CR2003272
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CE00082G
Abstract: Controlling the particle size of a flexible metal–organic framework demonstrates that a 2D to 3D transformation gives a kinetically-trapped, structurally-locked form.
Publisher: Wiley
Date: 20-07-2018
Abstract: The structural processing of metal-organic frameworks (MOFs) over multiple length scales is critical for their successful use as adsorbents in a variety of emerging applications. Although significant advances in molecular-scale design have provided strategies to boost the adsorptive capacities of MOFs, relatively little attention has been directed toward understanding the influence of higher-order structuralization on the material performance. Herein, we present the main strategies that are currently available for the structural processing of MOFs and discuss the influence these processes can impart on the adsorptive properties of the materials. In all, this intriguing area of research is expected to provide significant opportunities to enhance the properties of MOFs further, which will ultimately aid in their optimization in the context of specific real-world applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7TA02848B
Abstract: Addition of a modulator in the LPE process enhances MOF thin film properties by boosting their crystallinity, orientation uniformity, and adsorption capacity.
Publisher: American Chemical Society (ACS)
Date: 25-03-2011
DOI: 10.1021/JP200638N
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4CS00106K
Abstract: This review conceptually categorizes the available synthetic methodologies for structuring of MOFs in the mesoscopic and macroscopic scales.
Publisher: American Chemical Society (ACS)
Date: 10-01-2013
DOI: 10.1021/JA310173E
Abstract: Microporous metal-organic frameworks are a class of materials being vigorously investigated for mobile hydrogen storage applications. For high-pressure storage at ambient temperatures, the M(3)[(M(4)Cl)(3)(BTT)(8)](2) (M-BTT BTT(3-) = 1,3,5-benzenetristetrazolate) series of frameworks are of particular interest due to the high density of exposed metal cation sites on the pore surface. These sites give enhanced zero-coverage isosteric heats of adsorption (Q(st)) approaching the optimal value for ambient storage applications. However, the Q(st) parameter provides only a limited insight into the thermodynamics of the in idual adsorption sites, the tuning of which is paramount for optimizing the storage performance. Here, we begin by performing variable-temperature infrared spectroscopy studies of Mn-, Fe-, and Cu-BTT, allowing the thermodynamics of H(2) adsorption to be probed experimentally. This is complemented by a detailed DFT study, in which molecular fragments representing the metal clusters within the extended solid are simulated to obtain a more thorough description of the structural and thermodynamic aspects of H(2) adsorption at the strongest binding sites. Then, the effect of substitutions at the metal cluster (metal ion and anion within the tetranuclear cluster) is discussed, showing that the configuration of this unit indeed plays an important role in determining the affinity of the framework toward H(2). Interestingly, the theoretical study has identified that the Zn-based analogs would be expected to facilitate enhanced adsorption profiles over the compounds synthesized experimentally, highlighting the importance of a combined experimental and theoretical approach to the design and synthesis of new frameworks for H(2) storage applications.
Location: United States of America
Start Date: 2016
End Date: 12-2021
Amount: $373,536.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2019
End Date: 12-2021
Amount: $500,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 03-2022
End Date: 03-2025
Amount: $476,000.00
Funder: Australian Research Council
View Funded Activity