ORCID Profile
0000-0002-4663-7475
Current Organisations
University of Cambridge
,
University of Sydney
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Macromolecular and Materials Chemistry | Synthesis of Materials | Nanoscale Characterisation | Nanochemistry and Supramolecular Chemistry
Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in the Physical Sciences |
Publisher: Wiley
Date: 06-2020
Publisher: American Chemical Society (ACS)
Date: 02-06-2014
DOI: 10.1021/JA5042397
Abstract: We report the covalent post-assembly modification of kinetically metastable amine-bearing Fe(II)2L3 triple helicates via acylation and azidation. Covalent modification of the metastable helicates prevented their reorganization to the thermodynamically favored Fe(II)4L4 tetrahedral cages, thus trapping the system at the non-equilibrium helicate structure. This functionalization strategy also conveniently provides access to a higher-order tris(porphyrinatoruthenium)-helicate complex that would be difficult to prepare by de novo ligand synthesis.
Publisher: American Chemical Society (ACS)
Date: 04-01-2021
DOI: 10.26434/CHEMRXIV.13507446
Abstract: Self-immolative linkers offer efficient mechanisms for deprotecting ‘caged’ functional groups in response to specific stimuli. Herein we describe a convenient ‘click’ chemistry method for introducing pendant self-immolative linkers to a polymer backbone through post-polymerization modification. The intro duced triazole rings serve both to anchor the stimuli-cleavable trigger groups to the polymer backbone, while also forming a functional part of the self-immolation cascade. We investigate the polymerization kinetics, post-synthetic modification, and self-immolation mechanism of a model polymer system, and discuss avenues for future studies on poly-pendant self-immolative triazoles as a modular, stimuli-responsive macromolecule platform. / / /
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6TC02555B
Abstract: We report the synthesis and characterisation of novel copolymers comprising asymmetric perylene diimide acrylate monomers.
Publisher: Wiley
Date: 22-01-2021
Publisher: Wiley
Date: 08-05-2015
Publisher: Wiley
Date: 08-05-2015
Abstract: Copper(I) can preferentially form heteroleptic complexes containing two phosphine and two nitrogen donors due to steric factors. This preference was employed to direct the self-assembly of a porphyrin-faced rhomboidal prism having two parallel tetrakis(4-iminopyridyl)porphyrinatozinc(II) faces linked by eight 1,4-bis(diphenylphosphino)benzene pillars. The coordination preferences of the Cu(I) ions and geometries of the ligands come together to generate a slipped-cofacial orientation of the porphyrinatozinc(II) faces. This orientation enables selective encapsulation of 3,3'-bipyridine (bipy), which bridges the Zn(II) ions of the parallel porphyrins, whereas 4,4'-bipy exhibits weaker external coordination to the porphyrin faces. Reaction with 2,2'-bipy, by contrast, results in the displacement of the tetratopic porphyrin ligand and formation of [{(2,2'-bipy)Cu(I) }2 (diphosphine)2 ]. The differing strengths of interactions of bipyridine isomers with the system allows for a hierarchy to be deciphered, whereby 4,4'-bipy may be displaced by 3,3'-bipy, which in turn is displaced by 2,2'-bipy.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4PY00250D
Abstract: We report the synthesis and post-synthetic modification of a library of hydrophilic and hydrophobic ‘clicked’ triazole-linked porphyrin–polymer conjugates (PPCs), and their subsequent assembly into fluorescent bowl-shaped nanoparticles.
Publisher: Springer Science and Business Media LLC
Date: 21-08-2017
DOI: 10.1038/NCHEM.2839
Publisher: Wiley
Date: 12-08-2013
Abstract: The convergence of supramolecular chemistry and polymer science offers many powerful approaches for building functional nanostructures with well-defined dynamic behaviour. Herein we report the efficient "click" synthesis and self-assembly of AB2 - and AB4 -type multitopic porphyrin-polymer conjugates (PPCs). PPCs were prepared using the copper(I)-catalysed azide-alkyne cycloaddition (CuAAC) reaction, and consisted of linear polystyrene, poly(butyl acrylate), or poly(tert-butyl acrylate) arms attached to a zinc(II) porphyrin core via triazole linkages. We exploit the presence of the triazole groups obtained from CuAAC coupling to direct the self-assembly of the PPCs into short oligomers (2-6 units in length) via intermolecular porphyrinatozinc-triazole coordination. By altering the length and grafting density of the polymer arms, we demonstrate that the association constant of the porphyrinatozinc-triazole complex can be systematically tuned over two orders of magnitude. Self-assembly of the PPCs also resulted in a 6 K increase in the glass transition temperature of the bulk material compared to a non-assembling PPC. The modular synthesis and tunable self-assembly of the triazole-linked PPCs thus represents a powerful supramolecular platform for building functional nanostructured materials.
Publisher: Wiley
Date: 29-08-2022
Abstract: Polyurethane‐based hydrogels are relatively inexpensive and mechanically robust biomaterials with ideal properties for various applications, including drug delivery, prosthetics, implant coatings, soft robotics, and tissue engineering. In this report, a simple method is presented for synthesizing and casting biocompatible polyurethane‐poly(ethylene glycol) (PU‐PEG) hydrogels with tunable mechanical properties, nonfouling characteristics, and sustained tolerability as an implantable material or coating. The hydrogels are synthesized via a simple one‐pot method using commercially available precursors and low toxicity solvents and reagents, yielding a consistent and biocompatible gel platform primed for long‐term biomaterial applications. The mechanical and physical properties of the gels are easily controlled by varying the curing concentration, producing networks with complex shear moduli of 0.82–190 kPa, similar to a range of human soft tissues. When evaluated against a mechanically matched poly(dimethylsiloxane) (PDMS) formulation, the PU‐PEG hydrogels demonstrated favorable nonfouling characteristics, including comparable adsorption of plasma proteins (albumin and fibrinogen) and significantly reduced cellular adhesion. Moreover, preliminary murine implant studies reveal a mild foreign body response after 41 days. Due to the tunable mechanical properties, excellent biocompatibility, and sustained in vivo tolerability of these hydrogels, it is proposed that this method offers a simplified platform for fabricating soft PU‐based biomaterials for a variety of applications.
Publisher: American Chemical Society (ACS)
Date: 10-11-2015
DOI: 10.1021/JACS.5B09920
Abstract: Subcomponent self-assembly of two isomeric bis(3-aminophenyl)pyrenes, 2-formylpyridine and the metal ions Fe(II), Co(II), and Zn(II) led to the formation of two previously unidentified structure types: a C2-symmetric M(II)4L6 assembly with meridionally coordinated metal centers, and a C3-symmetric self-included M(II)4L6 assembly with facially coordinated metal centers. In both structures the meta linkages within the ligands facilitate π-stacking between the pyrene panels of the ligands. A C2h-symmetric M(II)2L2 box was also obtained, which was observed to selectively bind electron-deficient aromatic guests between two parallel pyrene subunits. Similar donor-acceptor interactions drove the selective self-assembly of a singular M(II)4L4L'2 architecture incorporating both a pyrene-containing diamine and an electron-deficient NDI-based diamine. This heteroleptic architecture was shown to be thermodynamically favored over the corresponding homoleptic M(II)4L6 and M(II)4L'6 complexes, which were nonetheless stable in each others' absence. By contrast, an isomeric pyrene-based diamine was observed to undergo narcissistic self-sorting in the presence of the NDI-based diamine.
Publisher: American Chemical Society (ACS)
Date: 23-07-2012
DOI: 10.1021/JP3043895
Abstract: We report the synthesis and ultrafast excited-state dynamics of two new meso-meso, β-β, β-β triply fused diporphyrins, Zn-3DP and Pd-3DP. Both compounds were found to have short excited-state lifetimes: Zn-3DP possessed an average S1 lifetime of 14 ps before nonradiative deactivation to the ground state, whereas Pd-3DP displayed a longer average S1 lifetime of 18 ps before crossing to the T1 state, which itself possessed a very short triplet lifetime of 1.7 ns. The excited-state dynamics of Zn-3DP, compared to similar zinc(II) diporphyrins reported in the literature, suggests that a conical intersection of the S1 and S0 potential energy surfaces plays a major role as a deactivation pathway of these molecules. Furthermore, the short triplet lifetime of Pd-3DP, compared to other diporphyrins that also exploit the intramolecular heavy atom effect, reveals that the position of the heavy atom within the diporphyrin framework influences the strength of spin-orbit coupling. The implications for employing triply fused diporphyrins as NIR-absorbing triplet sensitizers are discussed.
Publisher: American Chemical Society (ACS)
Date: 08-07-2018
DOI: 10.1021/JACS.8B05082
Abstract: Covalent post-assembly modification (PAM) reactions are useful synthetic tools for functionalizing and stabilizing self-assembled metal-organic complexes. Recently, PAM reactions have also been explored as stimuli for triggering supramolecular structural transformations. Herein we demonstrate the use of inverse electron-demand Diels-Alder (IEDDA) PAM reactions to induce supramolecular structural transformations starting from a tetrazine-edged Fe
Publisher: CSIRO Publishing
Date: 17-11-2021
DOI: 10.1071/CH21200
Abstract: Synthetic polymers are well known to self-assemble into a wide range of remarkable architectures with properties directly arising from their nanoscale morphologies. The rapid development of post-polymerisation modification reactions and techniques like polymerisation induced self-assembly (PISA) have fuelled new research into ‘smart’ polymer assemblies that can undergo well defined morphological transformations in response to external stimuli. These transformations can be used to modulate the properties of polymer assemblies in a ‘switchable’ fashion, offering great potential to generate smart materials that can dynamically adapt to changes in complex environments. This review aims to highlight key developments from the past five years in this rapidly evolving field, and we discuss innovations in polymer design, stimuli-responsivity mechanisms, transformation behaviours, and potential applications of shape-transformable polymeric nanostructures.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0SC00532K
Abstract: Triazole-based self-immolative linkers can be reversibly paused and restarted throughout their elimination cascades in response to environmental pH changes.
Publisher: American Chemical Society (ACS)
Date: 11-08-2015
DOI: 10.1021/JACS.5B05080
Abstract: Post-assembly modification (PAM) is a powerful tool for the modular functionalization of self-assembled structures. We report a new family of tetrazine-edged Fe(II)4L6 tetrahedral cages, prepared using different aniline subcomponents, which undergo rapid and efficient PAM by inverse electron-demand Diels-Alder (IEDDA) reactions. Remarkably, the electron-donating or -withdrawing ability of the para-substituent on the aniline moiety influences the IEDDA reactivity of the tetrazine ring 11 bonds away. This effect manifests as a linear free energy relationship, quantified using the Hammett equation, between σ(para) and the rate of the IEDDA reaction. The rate of PAM can thus be adjusted by varying the aniline subcomponent.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C6CS00907G
Abstract: This review examines the growing variety of covalent reactions used to achieve the post-assembly modification of self-assembled metallosupramolecular complexes.
Publisher: American Chemical Society (ACS)
Date: 08-04-2011
DOI: 10.1021/JZ200270W
Publisher: American Chemical Society (ACS)
Date: 21-03-2016
DOI: 10.1021/JACS.5B11831
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CS00165F
Abstract: This review discusses recent advances in the use of molecular containers in complex chemical systems, focusing on three aspects: host–guest behaviour, structural transformations and reactivity modulation.
Publisher: Wiley
Date: 27-09-2018
Abstract: We report a strategy for regulating the rate of internally bound anion exchange within an Fe
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5SC03926F
Abstract: Low-symmetry metal–organic architectures that feature unusual binding motifs are useful for exploring new modes of guest recognition.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1PY01169C
Abstract: Post-polymerization CuAAC reactions are used to ‘click’ stimuli-cleavable triazole end-caps onto self-immolative poly(ethyl glyoxylate).
Publisher: American Chemical Society (ACS)
Date: 17-01-2020
DOI: 10.26434/CHEMRXIV.10013078.V3
Abstract: The Cu(I)-catalyzed azide-alkyne ‘click’ reaction is used to generate triazole-based self-immolative linkers that can be reversibly paused and restarted throughout their elimination cascades. The formed 1,4-triazole ring expresses a pH-sensitive intermediate that can be switched dynamically between active and dormant states depending on the presence of acid or base, cleanly gating the release of payload in response to pH changes.
Publisher: American Chemical Society (ACS)
Date: 25-10-2019
DOI: 10.26434/CHEMRXIV.10013078.V1
Abstract: We describe the first report of a self-immolation cascade that can be reversibly paused and reactivated in response to pH changes. This system employs a triazole-based self-immolative linker, which expresses a pH-sensitive intermediate during its elimination sequence. This allows the system to respond to pH cues within its local environment, thus establishing a new way to gate self-immolative release using fluctuating or transient chemical signals.
Publisher: American Chemical Society (ACS)
Date: 25-10-2019
DOI: 10.26434/CHEMRXIV.10013078.V2
Abstract: We describe the first report of a self-immolation cascade that can be reversibly paused and reactivated in response to pH changes. This system employs a triazole-based self-immolative linker, which expresses a pH-sensitive intermediate during its elimination sequence. This allows the system to respond to pH cues within its local environment, thus establishing a new way to gate self-immolative release using fluctuating or transient chemical signals.
Publisher: American Chemical Society (ACS)
Date: 20-05-2016
DOI: 10.1021/JACS.6B02445
Abstract: Meridional (mer) coordination promotes the generation of larger and lower-symmetry prismatic metallosupramolecular structures, in contrast with the facial (fac) coordination common to smaller and higher-symmetry polyhedra. Here, we describe a general route to the selective formation of large metallosupramolecular prisms that contain exclusively mer-coordinated metal vertices. The use of 2-formylpyridine subcomponents that contain perfluorophenylene substituents at their 5-positions resulted in stereoselective formation of the iron(II) complexes from these subcomponents. Only mer vertices were observed, as opposed to the statistical fac/mer mixture otherwise generated. This mer-selective self-assembly could be used to prepare tetragonal (M8L12), pentagonal (M10L15), and hexagonal (M12L18) prisms by taking advantage of the subtle selectivities imposed by the different anilines and counterions employed. The equilibrium between the tetragonal and pentagonal prism followed a linear free-energy relationship, with the ratio between structures correlating with the Hammett σp(+) parameter of the incorporated aniline. The contrasting preferences of the fluorinated and nonfluorinated ligands to generate prisms and tetrahedra, respectively, were quantified energetically, with the destabilization increasing linearly for each "incorrect ligand" incorporated into either structure.
Publisher: American Chemical Society (ACS)
Date: 30-08-2011
DOI: 10.1021/JA206322N
Abstract: After benzene and naphthalene, the smallest polycyclic aromatic hydrocarbon bearing six-membered rings is the threefold-symmetric phenalenyl radical. Despite the fact that it is so fundamental, its electronic spectroscopy has not been rigorously scrutinized, in spite of growing interest in graphene fragments for molecular electronic applications. Here we used complementary laser spectroscopic techniques to probe the jet-cooled phenalenyl radical in vacuo. Its spectrum reveals the interplay between four electronic states that exhibit Jahn-Teller and pseudo-Jahn-Teller vibronic coupling. The coupling mechanism has been elucidated by the application of various ab initio quantum-chemical techniques.
Publisher: American Chemical Society (ACS)
Date: 17-01-2020
DOI: 10.26434/CHEMRXIV.10013078
Abstract: The Cu(I)-catalyzed azide-alkyne ‘click’ reaction is used to generate triazole-based self-immolative linkers that can be reversibly paused and restarted throughout their elimination cascades. The formed 1,4-triazole ring expresses a pH-sensitive intermediate that can be switched dynamically between active and dormant states depending on the presence of acid or base, cleanly gating the release of payload in response to pH changes. br
Publisher: American Chemical Society (ACS)
Date: 04-01-2021
DOI: 10.26434/CHEMRXIV.13507446.V1
Abstract: Self-immolative linkers offer efficient mechanisms for deprotecting ‘caged’ functional groups in response to specific stimuli. Herein we describe a convenient ‘click’ chemistry method for introducing pendant self-immolative linkers to a polymer backbone through post-polymerization modification. The intro duced triazole rings serve both to anchor the stimuli-cleavable trigger groups to the polymer backbone, while also forming a functional part of the self-immolation cascade. We investigate the polymerization kinetics, post-synthetic modification, and self-immolation mechanism of a model polymer system, and discuss avenues for future studies on poly-pendant self-immolative triazoles as a modular, stimuli-responsive macromolecule platform.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TC02457J
Abstract: Luminescent solar concentrators based on molecular dyes are a promising approach to light collection.
Publisher: Wiley
Date: 27-09-2018
Publisher: SPIE
Date: 19-08-2010
DOI: 10.1117/12.862739
Location: United Kingdom of Great Britain and Northern Ireland
Start Date: 2019
End Date: 2021
Funder: Australian Research Council
View Funded ActivityStart Date: 2017
End Date: 2019
Funder: European Commission
View Funded ActivityStart Date: 06-2019
End Date: 01-2022
Amount: $411,000.00
Funder: Australian Research Council
View Funded Activity