ORCID Profile
0000-0002-1093-8153
Current Organisation
Australian National University
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Research Topics
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.
Top 5 Research Topics
ANZSRC Field of Research (FoR)
Supramolecular chemistry | Transition Metal Chemistry | Macromolecular and Materials Chemistry | Macromolecular and materials chemistry | Nanochemistry and Supramolecular Chemistry
ANZSRC Socio-Economic Objective (SEO)
Expanding Knowledge in the Chemical Sciences | Solar-Photovoltaic Energy |
Related Links
Publications
A Switchable Palladium(II) Trefoil Entangled Tetrahedron with Temperature Dependence and Concentration Independence
Publisher: Wiley
Date: 23-08-2022
Abstract: Self‐assembly makes metallo‐interlocked architectures attractive targets, but being in equilibrium with smaller species means that they can suffer from dilution effects. We show that a junctioned system gives rise to a [Pd 4 (L) 2 ] 8+ trefoil entangled tetrahedron irrespective of concentration. Heating the s le reversibly shifts the equilibrium from the knot to an isomeric non‐interlocked dual metallo‐cycle, demonstrating that thermodynamic equilibria can still be exploited for switching even in the absence of concentration effects.
Heterometallic [MnPtn(L)2n]x+ Macrocycles from Dichloromethane-Derived Bis-2-pyridyl-1,2,3-triazole Ligands
Publisher: American Chemical Society (ACS)
Date: 18-08-2016
DOI: 10.1021/ACS.INORGCHEM.6B01435
Abstract: There is continued interest in the assembly of heterometallic metallosupramolecular assemblies due to the potential for new structural types and/or interesting chemical and physical properties. Two novel methylene-linked bis-2-pyridyl-1,2,3-triazole ligands (1a, 1b) were synthesized through CuAAC "click" chemistry between dichloromethane (DCM), sodium azide, and the appropriate ethynylpyridine, giving the shortest possible "regular" bis-pyridyl-1,2,3-triazole. The first ex le of bis-coordination of two 2-pyridyl-1,2,3-triazoles (Rpytri) around one Pt(II) center is reported, giving exclusive formation of head-to-tail [Pt(Rpytri)2](2+) complexes with vacant binding sites suitable for complexation with other metals and the formation of heterometallic assemblies. The concentration-dependent formation of an equilibrium mixture of a heterometallic [Pd2Pt2(L)4](8+) [4 + 4] square and [Pd3Pt3(L)6](12+) [6 + 6] hexagon was observed, and at lower concentrations ([reactants] = 1.5 mM) hexamer formation was negligible. The [Pt(L)2](2+) building block could also be utilized in the synthesis of a concentration-independent [Cu2Pt2(L)4](6+) metallomacrocyle. These compounds were characterized with (1)H, (13)C, and (1)H DOSY NMR spectroscopies, elemental analysis, mass spectrometry, and in some cases X-ray crystallography.
A Catalogue of Orthogonal Complementary Ligand Pairings for Palladium(II) Complexes
Publisher: Wiley
Date: 13-04-2022
Abstract: Molecular recognition is a form of information transfer, seen in the base pairing in DNA which is derived from the identity (acceptor or donor) and number of hydrogen bond sites within each base. Here we report bis ‐ligand palladium(II) complexes that exhibit similar complementarity. Pd(II) has square planar four‐coordinate geometry, giving control over ligand orientation and denticity. Pairings were developed using ligand denticity (3 : 1 or 2 : 2), and hydrogen bond capability (AA:DD or AD:DA) or lack thereof. Five pairings were investigated, with two sets of four being found fully orthogonal. The two 3 : 1 pairings exhibited limited ligand exchange. The extent of this exchange varied dependant on solvent from 2 : 1 (desired to undesired) to 6 : 1. A reliable and varied set of ligand pairs have therefore been developed for bis ‐ligand coordination sphere engineering in pursuit of sorting for complex molecular architectures and molecular‐level information storage and transfer events.
A Nona‐nuclear Heterometallic Pd 3 Pt 6 “Donut”‐Shaped Cage: Molecular Recognition and Photocatalysis
Publisher: Wiley
Date: 07-06-2018
Abstract: We report a simple, low-symmetry 2-(1-(pyridine-4-methyl)-1H-1,2,3-triazol-4-yl)pyridine ligand that has both monodentate and bidentate binding sites. With platinum(II) and/or palladium(II) ions, two ex les of a new nona-nuclear metallo-assembly have been accessed. These complexes were characterized by NMR spectroscopy, electrospray mass spectrometry (ESI-MS), and in key cases, X-ray crystallography. The cages possess three clefts comprised of planar cationic panels. This structural feature enables the binding of planar aromatic guests such as anthracene. More interestingly, the heterometallic assembly was able to catalyze the light-induced [4+2] cycloaddition of anthracene with singlet oxygen.
Reversible Transformation between a [PdL2]2+ “Figure‐of‐Eight” Complex and a [Pd2L2]4+ Dimer: Switching On and Off Self‐Recognition
Publisher: Wiley
Date: 09-01-2019
Abstract: Structural changes to metallosupramolecular assemblies resulting in the release or uptake of guests are currently well established, whereas transformations turning on and off specific self-recognition are far less developed. We report a novel ligand (2,6-bis(1-(3-pyridin-4-yl)phenyl-1H-1,2,3-triazol-4-yl)pyridine) possessing a tridentate central metal-binding site flanked by two pendant pyridyl arms. In a 2:1 ratio with Pd
Pho4 Is Essential for Dissemination of Cryptococcus neoformans to the Host Brain by Promoting Phosphate Uptake and Growth at Alkaline pH
Publisher: American Society for Microbiology
Date: 22-02-2017
Abstract: Cryptococcal meningitis is fatal without treatment and responsible for more than 500,000 deaths annually. To be a successful pathogen, C. neoformans must obtain an adequate supply of essential nutrients, including phosphate, from various host niches. Phosphate acquisition in fungi is regulated by the PHO signaling cascade, which is activated when intracellular phosphate decreases below a critical level. Induction of phosphate acquisition genes leads to the uptake of free phosphate via transporters. By blocking the PHO pathway using a Pho4 transcription factor mutant ( pho4Δ mutant), we demonstrate the importance of the pathway for cryptococcal dissemination and the establishment of brain infection in murine models. Specifically, we show that reduced dissemination of the pho4Δ mutant to the brain is due to an alkaline pH tolerance defect, as alkaline pH mimics the conditions of phosphate deprivation. The end result is inhibited proliferation in host tissues, particularly in blood.
Roles of Metal Ions in Foldamers and Other Conformationally Flexible Supramolecular Systems
Publisher: American Chemical Society (ACS)
Date: 22-08-2022
Exploiting Supramolecular Interactions to Control Isomer Distributions in Reduced-Symmetry [Pd2L4]4+ Cages
Publisher: American Chemical Society (ACS)
Date: 23-05-2022
DOI: 10.1021/ACS.INORGCHEM.2C00937
Abstract: High-symmetry metallosupramolecular architectures (MSAs) have been exploited for a range of applications including molecular recognition, catalysis, and drug delivery. Recently, there have been increasing efforts to enhance those applications by generating reduced-symmetry MSAs. Here we report our attempts to use supramolecular (dispersion and hydrogen-bonding) forces and solvophobic effects to generate isomerically pure [Pd
Quadruply Stranded Metallo-Supramolecular Helicate [Pd2(hextrz)4]4+ Acts as a Molecular Mimic of Cytolytic Peptides
Publisher: American Chemical Society (ACS)
Date: 29-04-2020
Stoichiometric Control of Guest Recognition of Self‐Assembled Palladium(II)‐Based Supramolecular Architectures
Publisher: Wiley
Date: 11-09-2023
Abstract: We report flexible [Pd(L)2]2+ complexes where there is self‐recognition, driven by π ‐ π interactions between electron‐rich aromatic arms and the cationic regions they are tethered to. This self‐recognition h ers the association of these molecules with aromatic molecular targets in solution. In one case, this complex can be reversibly converted to an ‘open’ [Pd2(L)2]4+ macrocycle through introduction of more metal ion. This is accomplished by the ligand having two bidentate binding sites: a 2‐pyridyl‐1,2,3‐triazole site, and a bis‐1,2,3‐triazole site. Due to favourable hydrogen bonding, the 2‐pyridyl‐1,2,3‐triazole units reliably coordinate in the [Pd(L)2]2+ complex to control speciation: a second equivalent of Pd(II) is required to enforce coordination to bis‐triazole sites and form the macrocycle. The macrocycle interacts with a molecular substrate with higher affinity. In this fashion we are able to use stoichiometry to reversibly switch between two different species and regulate guest binding.
Functional metallosupramolecular architectures using 1,2,3-triazole ligands: it's as easy as 1,2,3 “click”
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C6DT04702E
Abstract: Self-assembled metallosupramolecular architectures generated using “click” ligands have become an increasingly popular area of inorganic chemistry.
Self‐assembly and Cycling of a Three‐state Pd x L y Metallosupramolecular System
Publisher: Wiley
Date: 17-09-2019
Abstract: The use of stimuli to induce reversible structural transformations in metallosupramolecular systems is of keen interest to chemists seeking to mimic the way that Nature effects conformational changes in biological machinery. While a wide array of stimuli have been deployed towards this end, stoichiometric changes have only been explored in a handful of ex les. Furthermore, switching has generally been between only two distinct states. Here we use a simple 2-(1-(pyridine-4-methyl)-1H-1,2,3-triazol-4-yl)pyridine "click" ligand in combination with Pd
Synthesis, Characterisation and Antimicrobial Studies of some 2,6‐bis(1,2,3‐Triazol‐4‐yl)Pyridine Ruthenium(II) “Click” Complexes
Publisher: Wiley
Date: 21-03-2019
Discrete Self‐Assembled Metallo‐Foldamers with Heteroleptic Sequence Specificity
Publisher: Wiley
Date: 06-08-2021
Abstract: Discrete and structurally erse foldamer sequences are constructed in both natural and abiotic systems primarily using inert connectivity with irreversible organic covalent bonds, serving to preserve the identity of the sequence. The formation of sequences under thermodynamic control using labile coordination bonds would be attractive for synthetic ease and modular capability, but this presents issues regarding sequence preservation. Here is presented an approach integrating palladium(II) metal ions into the sequence itself, with fidelity maintained through use of complementary pairings of ligand arrangements at the metal centre. This is accomplished using sites of different denticity and/or hydrogen bonding capability. In this fashion, discrete and ordered metallo‐sequences are formed as thermodynamic products in a single step, and these then fold into defined conformations due to π–π interactions between electron‐rich and ‐poor aromatic regions of the combined componentry.
Oxidatively Locked [Co2L3]6+ Cylinders Derived from Bis(bidentate) 2-Pyridyl-1,2,3-triazole “Click” Ligands: Synthesis, Stability, and Antimicrobial Studies
Publisher: MDPI AG
Date: 16-11-2016
A Lantern‐Shaped Pd(II) Cage Constructed from Four Different Low‐Symmetry Ligands with Positional and Orientational Control: An Ancillary Pairings Approach
Publisher: Wiley
Date: 31-10-2023
Fungal physiology: Red light plugs into MAPK pathway.
Publisher: Springer Science and Business Media LLC
Date: 26-04-2016
Self-assembly with 2,6-Bis(1-(pyridin-4-ylmethyl)- 1H-1,2,3-triazol-4-yl)pyridine: Silver(I) and Iron(II) complexes
Publisher: MDPI AG
Date: 19-10-2017
Anticancer Activity and Cisplatin Binding Ability of Bis-Quinoline and Bis-Isoquinoline Derived [Pd2L4]4+ Metallosupramolecular Cages
Publisher: Frontiers Media SA
Date: 22-11-2018
Heterotrimetallic Double Cavity Cages: Syntheses and Selective Guest Binding
Publisher: Wiley
Date: 04-03-2022
Abstract: A strategy for the generation of heterotrimetallic double cavity (DC) cages [Pd n Pt m L 4 ] 6+ ( DC1 : n =1, m =2 and DC2 : n =2, m =1) is reported. The DC cages were generated by combining an inert platinum(II) tetrapyridylaldehyde complex with a suitably substituted pyridylamine and Pd II ions. 1 H and DOSY nuclear magnetic resonance spectroscopy (NMR) and electrospray ionization mass spectrometry (ESIMS) data were consistent with the formation of the DC architectures. DC1 and DC2 were shown to interact with several different guest molecules. The structure of DC1 , which features two identical cavities, binding two 2,6‐diaminoanthraquinone ( DAQ ) guest molecules was determined by single‐crystal X‐ray crystallography. In addition, DC1 was shown to bind two molecules of 5‐fluorouracil ( 5‐FU ) in a statistical (non‐cooperative) manner. In contrast, DC2 , which features two different cage cavities, was found to interact with two different guests, 5‐FU and cisplatin , selectively.
Untangling knotty problems
Publisher: Springer Science and Business Media LLC
Date: 29-01-2021
Regulatory mechanism of the atypical AP-1-like transcription factor yap1 in Cryptococcus neoformans
Publisher: American Society for Microbiology
Date: 18-12-2019
Abstract: The human meningitis fungal pathogen, Cryptococcus neoformans , contains the atypical yeast AP-1-like protein Yap1. Yap1 lacks an N-terminal cysteine-rich domain (n-CRD), which is present in other fungal Yap1 orthologs, but has a C-terminal cysteine-rich domain (c-CRD). However, the role of c-CRD and its regulatory mechanism remain unknown. Here, we report that Yap1 is transcriptionally regulated in response to oxidative, osmotic, and membrane-destabilizing stresses partly in an Mpk1-dependent manner, supporting its role in stress resistance. The c-CRD domain contributed to the role of Yap1 only in resistance to certain oxidative stresses and azole drugs but not in other cellular functions. Yap1 has a minor role in the survival of C. neoformans in a murine model of systemic cryptococcosis.
The TOR Pathway Plays Pleiotropic Roles in Growth and Stress Responses of the Fungal Pathogen Cryptococcus neoformans
Publisher: Oxford University Press (OUP)
Date: 07-06-2019
DOI: 10.1534/GENETICS.119.302191
Abstract: The target of rapamycin (TOR) pathway is an evolutionarily conserved signal transduction system that governs a plethora of eukaryotic biological processes, but its role in Cryptococcus neoformans remains elusive. In this study, we investigated the TOR pathway by functionally characterizing two Tor-like kinases, Tor1 and Tlk1, in C. neoformans. We successfully deleted TLK1, but not TOR1. TLK1 deletion did not result in any evident in vitro phenotypes, suggesting that Tlk1 is dispensable for the growth of C. neoformans. We demonstrated that Tor1, but not Tlk1, is essential and the target of rapamycin by constructing and analyzing conditionally regulated strains and sporulation analysis of heterozygous mutants in the diploid strain background. To further analyze the Tor1 function, we constructed constitutive TOR1 overexpression strains. Tor1 negatively regulated thermotolerance and the DNA damage response, which are two important virulence factors of C. neoformans. TOR1 overexpression reduced Mpk1 phosphorylation, which is required for cell wall integrity and thermoresistance, and Rad53 phosphorylation, which governs the DNA damage response pathway. Tor1 is localized to the cytoplasm, but enriched in the vacuole membrane. Phosphoproteomics and transcriptomics revealed that Tor1 regulates a variety of biological processes, including metabolic processes, cytoskeleton organization, ribosome biogenesis, and stress response. TOR inhibition by rapamycin caused actin depolarization in a Tor1-dependent manner. Finally, screening rapamycin-sensitive and -resistant kinase and transcription factor mutants revealed that the TOR pathway may crosstalk with a number of stress signaling pathways. In conclusion, our study demonstrates that a single Tor1 kinase plays pleiotropic roles in C. neoformans.
Functional metal complexes from CuAAC “click” bidentate and tridentate pyridyl-1,2,3-triazole ligands
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7DT04570K
Abstract: This Frontiers article examines the use of “click” complexes for the development of catalysts, anti-cancer and anti-bacterial agents and emissive materials.
Using Complementary Ligand Denticity to Direct Metallosupramolecular Structure about Metal Ions with Square‐Planar Geometry
Publisher: Wiley
Date: 03-2020
Exploiting reduced-symmetry ligands with pyridyl and imidazole donors to construct a second-generation stimuli-responsive heterobimetallic [PdPtL4]4+ cage
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC01354E
Abstract: A new method for the assembly of a heterobimetallic [PdPtL 4 ] 4+ cage which can interact with anionic guest molecules in a specific, selective host–guest orientation is described.
Solid-State Gas Adsorption Studies with Discrete Palladium(II) [Pd2(L)4]4+Cages
Publisher: Wiley
Date: 27-06-2017
Abstract: The need for effective CO
Directing metallo-supramolecular assembly through complementarity
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC04464A
Abstract: This Feature Article details our strategies using complementary pairs of ligands to control connectivity at metal ions and direct structure in metallo-supramolecular self-assembly.
Heteroleptic Tripalladium(II) Cages
Publisher: Wiley
Date: 21-02-2022
Abstract: There is a concerted attempt to develop self‐assembled metallo‐cages of greater structural complexity, and heteroleptic Pd II cages are emerging as prime candidates in these efforts. Most of these are dinuclear: few ex les of higher nuclearity have been reported. We demonstrate here a robust method for the formation of tripalladium(II) cages from the 2 : 3 : 3 combination of a tritopic ligand, Pd II , and a selection of ditopic ligands of the correct size and geometry.
A Lantern‐Shaped Pd(II) Cage Constructed from Four Different Low‐Symmetry Ligands with Positional and Orientational Control: An Ancillary Pairings Approach
Publisher: Wiley
Date: 31-10-2023
Strategies for Reversible Guest Uptake and Release from Metallosupramolecular Architectures
Publisher: Wiley
Date: 03-09-2018
Abstract: The cavities of metallosupramolecular cages can be used to mimic the central spaces of naturally occurring proteins and bind a wide variety of molecular guests. A range of potential applications have arisen from this capacity for host-guest chemistry. However, to truly harness the opportunities thus afforded, methodologies to controllably allow the release and reuptake of guests from the cavities of metallosupramolecular cages are required. Methods to accomplish this have centered upon reversibly altering the character of either the guest or host. This minireview outlines the current approaches used to carry out the binding and release of guests from metallosupramolecular hosts using important ex les from the field.
Inside Back Cover: Solid-State Gas Adsorption Studies with Discrete Palladium(II) [Pd2(L)4]4+ Cages (Chem. Eur. J. 44/2017)
Publisher: Wiley
Date: 27-06-2017
Long-cavity [Pd2L4]4+ cages and designer 1,8-naphthalimide sulfonate guests: rich variation in affinity and differentiated binding stoichiometry
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0QI00658K
Abstract: Long cavity dual domain [Pd 2 L 4 ] 4+ cages bind long, dual domain guests, with tunable binding affinities and stoichiometries.
Post‐Synthetic Modification of a Porous Hydrocarbon Cage to Give a Discrete Co24 Organometallic Complex**
Publisher: Wiley
Date: 21-07-2022
Abstract: A new alkyne‐based hydrocarbon cage was synthesized in high overall yield using alkyne‐alkyne coupling in the cage forming step. The cage is porous and displays a moderately high BET surface area (546 m 2 g −1 ). The cage loses crystallinity on activation and thus is porous in its amorphous form, while very similar cages have been either non‐porous, or retained crystallinity on activation. Reaction of the cage with Co 2 (CO) 8 results in exhaustive metalation of its 12 alkyne groups to give the Co 24 (CO) 72 adduct of the cage in good yield.
Exploiting the labile site in dinuclear [Pd2L2]n+ metallo-cycles: multi-step control over binding affinity without alteration of core host structure
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0QI00901F
Abstract: Synthetic metallosupramolecular systems have generally been binary (on/off) when they have control over molecular recognition. This report details a dipalladium( ii ) system with four-step graduated control over recognition for a guest.
Controlled Formation of Heteroleptic [Pd2 (La )2 (Lb )2 ]4+ Cages
Publisher: American Chemical Society (ACS)
Date: 12-08-2016
DOI: 10.1021/JACS.6B05629
Abstract: Metallosupramolecular architectures are beginning to be exploited for a range of applications including drug delivery, catalysis, molecular recognition, and sensing. For the most part these achievements have been made with high-symmetry metallosupramolecular architectures composed of just one type of ligand and metal ion. Recently, considerable efforts have been made to generate metallosupramolecular architectures that are made up of multiple different ligands and/or metals ions in order to obtain more complex systems with new properties. Herein we show that the addition of an electron-rich 2-amino-substituted tripyridyl ligand, 2,6-bis(pyridin-3-ylethynyl)pyridine (2A-tripy), to a solution of the [Pd2(tripy)4](4+) cage resulted in the clean generation of a heteroleptic [Pd2(tripy)2(2A-tripy)2](4+) architecture. The formation of the mixed-ligand cage [Pd2(tripy)2(2A-tripy)2](4+) was confirmed using (1)H NMR spectroscopy, diffusion-ordered spectroscopy, and rotating-frame nuclear Overhauser effect spectroscopy and high-resolution electrospray ionization mass spectrometry. Density functional theory calculations suggested the cis isomer was more stable that the trans isomer. Additionally, the calculations indicated that the heteroleptic palladium(II) cages are kinetically metastable intermediates rather than the thermodynamic product of the reaction. Competition experiments supported that finding and showed the cages are long-lived in solution at room temperature. Finally, it was shown that the addition of 2A-tripy to a range of preformed [Pd2(Ltripy)4](4+) cages cleanly generated the mixed-ligand systems. Three other systems displaying different exo and endo functionalities within the cage assembly were generated, suggesting that this method could be applied to synthesize a range of highly functionalized heteroleptic cis-[Pd2(La)2(Lb)2](4+) cages.
Induction of virus resistance by exogenous application of double-stranded RNA
Publisher: Elsevier BV
Date: 10-2017
DOI: 10.1016/J.COVIRO.2017.07.009
Abstract: Exogenous application of double-stranded RNA (dsRNA) for virus resistance in plants represents a very attractive alternative to virus resistant transgenic crops or pesticides targeting virus vectors. However, the instability of dsRNA sprayed onto plants is a major challenge as spraying naked dsRNA onto plants provides protection against homologous viruses for only 5 days. Innovative approaches, such as the use of nanoparticles as carriers of dsRNA for improved stability and sustained release, are emerging as key disruptive technologies. Knowledge is still limited about the mechanism of entry, transport and processing of exogenously applied dsRNA in plants. Cost of dsRNA and regulatory framework will be key influencers towards practical adoption of this technology.
Excited-State Switching in Rhenium(I) Bipyridyl Complexes with Donor–Donor and Donor–Acceptor Substituents
Publisher: American Chemical Society (ACS)
Date: 11-06-2021
DOI: 10.1021/JACS.1C02755
A Nona‐nuclear Heterometallic Pd3Pt6 “Donut”‐Shaped Cage: Molecular Recognition and Photocatalysis
Publisher: Wiley
Date: 07-06-2018
Frontispiece: Strategies for Reversible Guest Uptake and Release from Metallosupramolecular Architectures
Publisher: Wiley
Date: 09-10-2018
A symmetry interaction approach to [M2L2]4+ metallocycles and their self-catenation
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9CC07130J
Abstract: A symmetry interaction approach to [M 2 L 2 ] 4+ metallocycles and their self-catenanes.
A Dinuclear Platinum(II) N4Py Complex: An Unexpected Coordination Mode For N4Py
Publisher: American Chemical Society (ACS)
Date: 30-06-2015
DOI: 10.1021/ACS.INORGCHEM.5B01032
Abstract: The polypyridyl compound N,N-bis(2-pyridylmethyl)-N-bis(2-pyridyl)methylamine (N4Py) acts as a bridging ligand and coordinates to two Pt(II) ions giving an unexpected diplatinum(II) complex, whose photophysical and anticancer properties were investigated.
Heterotrimetallic Double Cavity Cages: Syntheses and Selective Guest Binding
Publisher: Wiley
Date: 04-03-2022
Abstract: A strategy for the generation of heterotrimetallic double cavity (DC) cages [Pd n Pt m L 4 ] 6+ ( DC1 : n =1, m =2 and DC2 : n =2, m =1) is reported. The DC cages were generated by combining an inert platinum(II) tetrapyridylaldehyde complex with a suitably substituted pyridylamine and Pd II ions. 1 H and DOSY nuclear magnetic resonance spectroscopy (NMR) and electrospray ionization mass spectrometry (ESIMS) data were consistent with the formation of the DC architectures. DC1 and DC2 were shown to interact with several different guest molecules. The structure of DC1 , which features two identical cavities, binding two 2,6‐diaminoanthraquinone ( DAQ ) guest molecules was determined by single‐crystal X‐ray crystallography. In addition, DC1 was shown to bind two molecules of 5‐fluorouracil ( 5‐FU ) in a statistical (non‐cooperative) manner. In contrast, DC2 , which features two different cage cavities, was found to interact with two different guests, 5‐FU and cisplatin , selectively.
Hydrazone- and imine-containing [PdPtL4]4+ cages: a comparative study of the stability and host–guest chemistry
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2DT02720H
Abstract: A new [PdPtL 4 ] 4+ heterobimetallic cage containing hydrazone linkages has been synthesised using the sub-component self-assembly approach.
Investigating the cytotoxicity of platinum(II) complexes incorporating bidentate pyridyl-1,2,3-triazole click ligands.
Publisher: Elsevier BV
Date: 12-2016
DOI: 10.1016/J.JINORGBIO.2016.06.017
Abstract: Six platinum(II) complexes of the type [Pt(P
A Switchable Palladium(II) Trefoil Entangled Tetrahedron with Temperature Dependence and Concentration Independence
Publisher: Wiley
Date: 23-08-2022
Abstract: Self‐assembly makes metallo‐interlocked architectures attractive targets, but being in equilibrium with smaller species means that they can suffer from dilution effects. We show that a junctioned system gives rise to a [Pd 4 (L) 2 ] 8+ trefoil entangled tetrahedron irrespective of concentration. Heating the s le reversibly shifts the equilibrium from the knot to an isomeric non‐interlocked dual metallo‐cycle, demonstrating that thermodynamic equilibria can still be exploited for switching even in the absence of concentration effects.
Multicavity [PdnL4]2n+ Cages with Controlled Segregated Binding of Different Guests
Publisher: American Chemical Society (ACS)
Date: 07-02-2017
DOI: 10.1021/JACS.6B11982
Abstract: Multicavity [Pd
Cover Feature: (ChemPlusChem 5/2020)
Publisher: Wiley
Date: 14-04-2020
Biologically active [Pd2L4]4+ quadruply-stranded helicates: stability and cytotoxicity
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5DT01259G
Abstract: A quadruply-stranded dipalladium( ii ) helicate exhibits low micromolar IC 50 values against a range of different cancer cell lines. Preliminary mechanistic studies indicate that the helicate induces cell death by disrupting the cell membrane.
Metallosupramolecular Architectures Formed with Ferrocene-Linked Bis-Bidentate Ligands: Synthesis, Structures, and Electrochemical Studies
Publisher: American Chemical Society (ACS)
Date: 30-01-2018
DOI: 10.1021/ACS.INORGCHEM.7B02503
Abstract: The self-assembly of ligands of different geometries with metal ions gives rise to metallosupramolecular architectures of differing structural types. The rotational flexibility of ferrocene allows for conformational ersity, and, as such, self-assembly processes with 1,1'-disubstituted ferrocene ligands could lead to a variety of interesting architectures. Herein, we report a small family of three bis-bidentate 1,1'-disubstituted ferrocene ligands, functionalized with either 2,2'-bipyridine or 2-pyridyl-1,2,3-triazole chelating units. The self-assembly of these ligands with the (usually) four-coordinate, diamagnetic metal ions Cu(I), Ag(I), and Pd(II) was examined using a range of techniques including
Dramatic Alteration of 3ILCT Lifetimes Using Ancillary Ligands in [Re(L)(CO)3(phen-TPA)]n+ Complexes: An Integrated Spectroscopic and Theoretical Study
Publisher: American Chemical Society (ACS)
Date: 14-03-2018
DOI: 10.1021/JACS.7B12868
Abstract: The ground and excited state photophysical properties of a series of fac-[Re(L)(CO)
Enhanced kinetic stability of [Pd2L4]4+ cages through ligand substitution
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6DT00133E
Abstract: [Pd 2 ( tripy ) 4 ] 4+ cage architectures (where tripy = 2,6-bis(pyridin-3-ylethynyl)pyridine) were made more kinetically robust in the presence of range of nucleophiles by the addition of amino groups in either the 2-( 2A-tripy ) or 3-( 3A-tripy ) positions of the tripy ligands' terminal pyridines, with the [Pd 2 ( 2A-tripy ) 4 ] 4+ cage proving the most stable.
Excited-State Switching Frustrates the Tuning of Properties in Triphenylamine-Donor-Ligand Rhenium(I) and Platinum(II) Complexes
Publisher: American Chemical Society (ACS)
Date: 27-04-2020
Multicavity Metallosupramolecular Architectures
Publisher: Wiley
Date: 14-09-2017
Abstract: Discrete metallosupramolecular systems are often macrocyclic or cage-like architectures with an accessible internal cavity. Guest molecules can reside within these cavities and much of the interest in these systems is derived from these fascinating host-guest interactions. A range of potential applications stem from the ability of these metallosupramolecular architectures to encapsulate guests. These applications include catalysis or acting as molecular reaction flasks, the molecular scavenging of pollutants, storage of reactive species, and drug delivery. Multicavity metallosupramolecular architectures combine the ability of large hollow assemblies to bind multiple guests concurrently with the binding specificity associated with small cages. A variety of different approaches to generating separate compartments within a single metallosupramolecular assembly have emerged. These include interpenetrated cages, cages with polytopic ligands that have a long backbone, and molecules that have two or more clefts. This review examines these approaches, and highlights key contributions to the field.
Chloride triggered reversible switching from a metallosupramolecular [Pd2 L4 ]4+ cage to a [Pd2 L2 Cl4 ] metallo-macrocycle with release of endo- and exo-hedrally bound guests
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5CC02226F
Abstract: A metallosupramolecular [Pd 2 L 4 ] 4+ cage can be cleanly, and reversibly, converted into a [Pd 2 L 2 Cl 4 ] metallo-macrocycle upon addition or removal of chloride ions.
Discrete Self‐Assembled Metallo‐Foldamers with Heteroleptic Sequence Specificity
Publisher: Wiley
Date: 06-08-2021
Abstract: Discrete and structurally erse foldamer sequences are constructed in both natural and abiotic systems primarily using inert connectivity with irreversible organic covalent bonds, serving to preserve the identity of the sequence. The formation of sequences under thermodynamic control using labile coordination bonds would be attractive for synthetic ease and modular capability, but this presents issues regarding sequence preservation. Here is presented an approach integrating palladium(II) metal ions into the sequence itself, with fidelity maintained through use of complementary pairings of ligand arrangements at the metal centre. This is accomplished using sites of different denticity and/or hydrogen bonding capability. In this fashion, discrete and ordered metallo‐sequences are formed as thermodynamic products in a single step, and these then fold into defined conformations due to π–π interactions between electron‐rich and ‐poor aromatic regions of the combined componentry.
Recognition Properties and Self‐assembly of Planar [M(2‐pyridyl‐1,2,3‐triazole)2]2+ Metallo‐ligands
Publisher: Wiley
Date: 20-09-2019
Abstract: Molecular recognition continues to be an area of keen interest for supramolecular chemists. The investigated [M(L)
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Related Funding Activities
Building Bigger And Better Cages: A Novel Approach To Large And Complex Molecules
Start Date: 2018
End Date: 2020
Funder: Rutherford Foundation Postdoctoral Fellowship
View Funded ActivityARC Future Fellowships - Grant ID: FT230100126
Start Date: 07-2023
End Date: 06-2027
Amount: $835,280.00
Funder: Australian Research Council
View Funded ActivityDiscovery Early Career Researcher Award - Grant ID: DE200100421
Start Date: 04-2020
End Date: 10-2023
Amount: $427,116.00
Funder: Australian Research Council
View Funded Activity