ORCID Profile
0000-0001-6373-4253
Current Organisations
Australian National University
,
Griffith University
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Publisher: American Chemical Society (ACS)
Date: 08-07-2014
DOI: 10.1021/JA504835A
Abstract: A new robust and high-yielding synthesis of the valuable U(III) synthon [U(BH4)3(THF)2] is reported. Reactivity in ligand exchange reactions is found to contrast significantly to that of uranium triiodide. This is exemplified by the synthesis and characterization of azamacrocyclic U(III) complexes, including mononuclear [U(BH4)(L)] and dinuclear [Li(THF)4][{U(BH4)}2(μ-BH4)(L(Me))] and [Na(THF)4][{U(BH4)}2(μ-BH4)(L(A))(THF)2]. The structures of all complexes have been determined by single-crystal X-ray diffraction and display two new U(III)2(BH4)3 motifs.
Publisher: Wiley
Date: 21-12-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7DT00327G
Abstract: The first structurally characterised chelated, saturated bis(NHC) complexes are reported along with facile ligand fragmentations during their synthesis.
Publisher: American Chemical Society (ACS)
Date: 18-12-2016
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8DT04116D
Abstract: Novel bis(2,9-diaryl-1,10-phenanthroline)copper( i ) complexes were prepared to study a photoredox-catalysed reaction.
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2DT11737A
Abstract: A range of aryloxy and alkoxy ligands, both monodenate and chelating, have been coordinated to Ti(IV) to yield complexes of the form [Ti(OAr)(2)Cl(2)], [Ti(RO^O)Cl(3)] and [Ti(RO^O)(2)Cl(2)] (R = aryl, alkyl). The complexes vary in their Lewis base solvation and/or aggregation state, as revealed by X-ray crystallography of selected ex les. The complexes have been evaluated as catalysts for ethylene oligomerisation and polymerisation following activation with alkylaluminium reagents (AlEt(3), methylaluminoxane). While polyethylene is the major product, ethylene oligomers also result, ranging from dimers to higher oligomers. The results indicate a number of different active species are formed upon activation, with oligomers likely arising through a metallacyclic mechanism. The findings are discussed in the context of the commercial Alphabutol dimerisation system [Ti(OR)(4)], and the development of group 4 based ethylene trimerisation catalysts.
Publisher: American Chemical Society (ACS)
Date: 16-02-2007
DOI: 10.1021/OM061143I
Publisher: American Chemical Society (ACS)
Date: 08-2008
DOI: 10.1021/OM800398E
Publisher: MDPI AG
Date: 07-05-2018
DOI: 10.20944/PREPRINTS201805.0118.V1
Abstract: The current report contributes to the understanding of the stereoselectivity of the chiral dirhodium(II) carboxylate catalysts derived from N-protected amino acid ligands. Investigating the possible effect of ligand stereo-purity on catalyst structure and enantioselectivity was carried out. This was justified through a new X-ray crystal structure for Rh2(S,S,S,R-PTTL)4 diastereomer.
Publisher: American Chemical Society (ACS)
Date: 20-01-2015
DOI: 10.1021/OM5012193
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3DT32183E
Abstract: A range of unsubstituted (1,2) and 6-substituted (3-5) ortho-phenoxy-imine ligands have been prepared and converted to their silyl ether derivatives (6-10). Reaction of silyl ethers with TiCl(4)(thf)(2) in the case of the unsubstituted species yields bis-ligated complexes while the substituted species react cleanly to yield complexes of the form [Ti(O^NR)Cl(3)(thf)]. In most cases the complexes have been characterised by X-ray crystallography. Testing of the complexes for ethylene oligomerisation and polymerisation has been undertaken employing alkylaluminium co-catalysts (AlEt(3), MAO). In all cases the predominant product formed is polyethylene however careful analysis of the liquid phase reveals a complex process by which 1-butene is most likely formed via Cossee mechanism while 1-hexene results from a metallacyclic process.
Publisher: Wiley
Date: 13-03-2020
Abstract: The most pressing challenges for light‐driven hydrogel actuators include reliance on UV light, slow response, poor mechanical properties, and limited functionalities. Now, a supramolecular design strategy is used to address these issues. Key is the use of a benzylimine‐functionalized anthracene group, which red‐shifts the absorption into the visible region and also stabilizes the supramolecular network through π–π interactions. Acid–ether hydrogen bonds are incorporated for energy dissipation under mechanical deformation and maintaining hydrophilicity of the network. This double‐crosslinked supramolecular hydrogel developed via a simple synthesis exhibits a unique combination of high strength, rapid self‐healing, and fast visible‐light‐driven shape morphing both in the wet and dry state. As all of the interactions are dynamic, the design enables the structures to be recycled and reprogrammed into different 3D objects.
Publisher: Springer Science and Business Media LLC
Date: 23-05-2016
DOI: 10.1038/NCHEM.2520
Abstract: Studies of transuranic organometallic complexes provide a particularly valuable insight into covalent contributions to the metal-ligand bonding, in which the subtle differences between the transuranium actinide ions and their lighter lanthanide counterparts are of fundamental importance for the effective remediation of nuclear waste. Unlike the organometallic chemistry of uranium, which has focused strongly on U(III) and has seen some spectacular advances, that of the transuranics is significantly technically more challenging and has remained dormant. In the case of neptunium, it is limited mainly to Np(IV). Here we report the synthesis of three new Np(III) organometallic compounds and the characterization of their molecular and electronic structures. These studies suggest that Np(III) complexes could act as single-molecule magnets, and that the lower oxidation state of Np(II) is chemically accessible. In comparison with lanthanide analogues, significant d- and f-electron contributions to key Np(III) orbitals are observed, which shows that fundamental neptunium organometallic chemistry can provide new insights into the behaviour of f-elements.
Publisher: Springer Science and Business Media LLC
Date: 21-05-2020
DOI: 10.1038/S41467-020-15706-X
Abstract: The electrocardiographic PR interval reflects atrioventricular conduction, and is associated with conduction abnormalities, pacemaker implantation, atrial fibrillation (AF), and cardiovascular mortality. Here we report a multi-ancestry ( N = 293,051) genome-wide association meta-analysis for the PR interval, discovering 202 loci of which 141 have not previously been reported. Variants at identified loci increase the percentage of heritability explained, from 33.5% to 62.6%. We observe enrichment for cardiac muscle developmental/contractile and cytoskeletal genes, highlighting key regulation processes for atrioventricular conduction. Additionally, 8 loci not previously reported harbor genes underlying inherited arrhythmic syndromes and/or cardiomyopathies suggesting a role for these genes in cardiovascular pathology in the general population. We show that polygenic predisposition to PR interval duration is an endophenotype for cardiovascular disease, including distal conduction disease, AF, and atrioventricular pre-excitation. These findings advance our understanding of the polygenic basis of cardiac conduction, and the genetic relationship between PR interval duration and cardiovascular disease.
Publisher: CSIRO Publishing
Date: 2010
DOI: 10.1071/CH10006
Abstract: Structural analogues of the phytotoxic thaxtomin natural products have been synthesized by building upon a piperazinedione core and from l-phenylalanine. The compounds were evaluated for their phytotoxic activity against Arabidopsis thaliana seedlings and some of the key features for activity have been identified.
Publisher: Elsevier BV
Date: 08-2018
Publisher: Springer Science and Business Media LLC
Date: 25-09-2020
DOI: 10.1186/S13073-020-00779-6
Abstract: Systemic sclerosis (SSc) is a genetically complex autoimmune disease mediated by the interplay between genetic and epigenetic factors in a multitude of immune cells, with CD4+ T lymphocytes as one of the principle drivers of pathogenesis. DNA s les exacted from CD4+ T cells of 48 SSc patients and 16 healthy controls were hybridized on MethylationEPIC BeadChip array. In parallel, gene expression was interrogated by hybridizing total RNA on Clariom™ S array. Downstream bioinformatics analyses were performed to identify correlating differentially methylated CpG positions (DMPs) and differentially expressed genes (DEGs), which were then confirmed utilizing previously published promoter capture Hi-C (PCHi-C) data. We identified 9112 and 3929 DMPs and DEGs, respectively. These DMPs and DEGs are enriched in functional categories related to inflammation and T cell biology. Furthermore, correlation analysis identified 17,500 possible DMP-DEG interaction pairs within a window of 5 Mb, and utilizing PCHi-C data, we observed that 212 CD4+ T cell-specific pairs of DMP-DEG also formed part of three-dimensional promoter-enhancer networks, potentially involving CTCF. Finally, combining PCHi-C data with SSc GWAS data, we identified four important SSc-associated susceptibility loci, TNIP1 (rs3792783), GSDMB (rs9303277), IL12RB1 (rs2305743), and CSK (rs1378942), that could potentially interact with DMP-DEG pairs cg17239269- ANXA6 , cg19458020- CCR7 , cg10808810- JUND , and cg11062629- ULK3 , respectively. Our study unveils a potential link between genetic, epigenetic, and transcriptional deregulation in CD4+ T cells of SSc patients, providing a novel integrated view of molecular components driving SSc pathogenesis.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5CE00375J
Abstract: Di(2-pyridylmethyl)amine carboxylates with short alkyl linkers afford coordination polymers whereas the longer homologues favour macrocyclic topologies.
Publisher: BMJ
Date: 04-2021
DOI: 10.1136/ANNRHEUMDIS-2021-219884
Abstract: The greatest genetic effect reported for systemic sclerosis (SSc) lies in the major histocompatibility complex (MHC) locus. Leveraging the largest SSc genome-wide association study, we aimed to fine-map this region to identify novel human leucocyte antigen (HLA) genetic variants associated with SSc susceptibility and its main clinical and serological subtypes. 9095 patients with SSc and 17 584 controls genome-wide genotyped were used to impute and test single-nucleotide polymorphisms (SNPs) across the MHC, classical HLA alleles and their composite amino acid residues. Additionally, patients were stratified according to their clinical and serological status, namely, limited cutaneous systemic sclerosis (lcSSc), diffuse cutaneous systemic sclerosis (dcSSc), anticentromere (ACA), antitopoisomerase (ATA) and anti-RNApolIII autoantibodies (ARA). Sequential conditional analyses showed nine SNPs, nine classical alleles and seven amino acids that modelled the observed associations with SSc. This confirmed previously reported associations with HLA-DRB1*11:04 and HLA-DPB1*13:01 , and revealed a novel association of HLA-B*08:01 . Stratified analyses showed specific associations of HLA-DQA1*02:01 with lcSSc, and an exclusive association of HLA-DQA1*05:01 with dcSSc. Similarly, private associations were detected in HLA-DRB1*08:01 and confirmed the previously reported association of HLA-DRB1*07:01 with ACA-positive patients, as opposed to the HLA-DPA1*02:01 and HLA-DQB1*03:01 alleles associated with ATA presentation. This study confirms the contribution of HLA class II and reveals a novel association of HLA class I with SSc, suggesting novel pathways of disease pathogenesis. Furthermore, we describe specific HLA associations with SSc clinical and serological subtypes that could serve as biomarkers of disease severity and progression.
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2DT31086D
Abstract: Synthetic routes to methyl(aryl)alkynylpalladium(IV) motifs are presented, together with studies of selectivity in carbon-carbon coupling by reductive elimination from Pd(IV) centres. The iodonium reagents IPh(C≡CR)(OTf) (R = SiMe(3), Bu(t), OTf = O(3)SCF(3)) oxidise Pd(II)Me(p-Tol)(L(2)) (1-3) [L(2) = 1,2-bis(dimethylphosphino)ethane (dmpe) (1), 2,2'-bipyridine (bpy) (2), 1,10-phenanthroline (phen) (3)] in acetone-d(6) or toluene-d(9) at -80 °C to form complexes Pd(IV)(OTf)Me(p-Tol)(C≡CR)(L(2)) [R = SiMe(3), L(2) = dmpe (4), bpy (5), phen (6) R = Bu(t), L(2) = dmpe (7), bpy (8), phen (9)] which reductively eliminate predominantly (>90%) p-Tol-C≡CR above ~-50 °C. NMR spectra show that isomeric mixtures are present for the Pd(IV) complexes: three for dmpe complexes (4, 7), and two for bpy and phen complexes (5, 6, 8, 9), with reversible reduction in the number of isomers to two occurring between -80 °C and -60 °C observed for the dmpe complex 4 in toluene-d(8). Kinetic data for reductive elimination from Pd(IV)(OTf)Me(p-Tol)(C≡CSiMe(3))(dmpe) (4) yield similar activation parameters in acetone-d(6) (66 ± 2 kJ mol(-1), ΔH(‡) 64 ± 2 kJ mol(-1), ΔS(‡)-67 ± 2 J K(-1) mol(-1)) and toluene-d(8) (E(a) 68 ± 3 kJ mol(-1), ΔH(‡) 66 ± 3 kJ mol(-1), ΔS(‡)-74 ± 3 J K(-1) mol(-1)). The reaction rate in acetone-d(6) is unaffected by addition of sodium triflate, indicative of reductive elimination without prior dissociation of triflate. DFT computational studies at the B97-D level show that the energy difference between the three isomers of 4 is small (12.6 kJ mol(-1)), and is similar to the energy difference encompassing the six potential transition state structures from these isomers leading to three feasible C-C coupling products (13.0 kJ mol(-1)). The calculations are supportive of reductive elimination occurring directly from two of the three NMR observed isomers of 4, involving lower activation energies to form p-TolC≡CSiMe(3) and earlier transition states than for other products, and involving coupling of carbon atoms with higher s character of σ-bonds (sp(2) for p-Tol, sp for C≡C-SiMe(3)) to form the product with the strongest C-C bond energy of the potential coupling products. Reductive elimination occurs predominantly from the isomer with Me(3)SiC≡C trans to OTf. Crystal structure analyses are presented for Pd(II)Me(p-Tol)(dmpe) (1), Pd(II)Me(p-Tol)(bpy) (2), and the acetonyl complex Pd(II)Me(CH(2)COMe)(bpy) (11).
Publisher: Informa UK Limited
Date: 07-2005
Publisher: Bentham Science Publishers Ltd.
Date: 07-2012
Publisher: American Chemical Society (ACS)
Date: 19-08-2020
DOI: 10.26434/CHEMRXIV.12812000.V1
Abstract: Despite their apparent similarity, framework materials based on tetraphenylmethane and tetraphenylsilane building blocks often have quite different structures and topologies. Herein, we describe a new silicon tetraamidinium compound and use it to prepare crystalline hydrogen bonded frameworks with carboxylate anions in water. The silicon-containing frameworks are compared with those prepared from the analogous carbon tetraamidinium: when biphenyldicarboxylate or tetrakis(4-carboxyphenyl)methane anions were used similar channel-containing networks are observed for both the silicon and carbon tetraamidinium. When terephthalate or bicarbonate anions were used, different products form. Insights into possible reasons for the different products are provided by a survey of the Cambridge Structural Database and quantum chemical calculations, both of which indicate that, contrary to expectations, tetraphenylsilane derivatives have less geometrical flexibility than tetraphenylmethane derivatives, i.e. they are less able to distort away from ideal tetrahedral bond angles.
Publisher: Wiley
Date: 16-01-2019
Publisher: Wiley
Date: 05-10-2017
Abstract: Four planar tripyridyl ligands (L
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6OB90061E
Abstract: Correction for ‘Oxidative ring-opening of ferrocenylcyclopropylamines to N -ferrocenylmethyl β-hydroxyamides’ by Yi Sing Gee et al. , Org. Biomol. Chem. , 2016, 14 , 2498–2503.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5DT03257A
Abstract: The insertion of internal olefins and chain walking isomerisation at di- n -octylaluminium hydride [Al(Oct) 2 H], promoted by zirconocene dichloride [Cp 2 ZrCl 2 ] has been studied.
Publisher: Elsevier BV
Date: 02-2008
Publisher: American Chemical Society (ACS)
Date: 05-06-2008
DOI: 10.1021/OM800122K
Publisher: Royal Society of Chemistry (RSC)
Date: 2005
DOI: 10.1039/B417679K
Abstract: The gamma-deprotonation of a samarium(III) bis(trimethylsilyl)amide complex derived from a dimetallated trans-dioxaporphyrinogen has been achieved through stabilisation of the counter cation within the macrocyclic cavity.
Publisher: International Union of Crystallography (IUCr)
Date: 08-12-2007
Publisher: American Chemical Society (ACS)
Date: 08-05-2012
DOI: 10.1021/OM2011134
Publisher: Wiley
Date: 19-08-2010
Publisher: American Chemical Society (ACS)
Date: 27-04-2016
DOI: 10.1021/ACS.INORGCHEM.5B02602
Abstract: The synthesis of two bipyridine-hexa-peri-hexabenzocoronene (bpy-HBC) ligands functionalized with either (t)Bu or C12H25 and their Re(I) tricarbonyl chloride complexes are reported and their electronic properties investigated using spectroscopic and computational methods. The metal complexes show unusual properties, and we observed the formation of a long-lived excited state using time-resolved infrared spectroscopy. Depending on the solvent, this appears to be of the form Rebpy(•-)HBC(•+) or a bpy-centered π,π* state. TD-DFT calculations support the donor-acceptor charge transfer character of these systems, in which HBC is the donor and bpy is the acceptor. The ground state optical properties are dominated by the HBC chromophore with additional distinct transitions of the complexes, one associated with MLCT 450 nm (ε > 17 000 L mol(-1) cm(-1)) and another with a HBC/metal to bpy charge transfer, termed the MLLCT band (373 nm, ε = 66 000 L mol(-1) cm(-1)). These assignments are also supported by resonance Raman spectroscopy.
Publisher: American Chemical Society (ACS)
Date: 06-04-2005
DOI: 10.1021/OM050172A
Publisher: American Chemical Society (ACS)
Date: 23-12-2022
DOI: 10.1021/ACS.INORGCHEM.1C03336
Abstract: A range of palladium complexes featuring electronically modified, imidazole-based abnormal N-heterocyclic carbene (aNHC) ligands have been prepared in the hopes of accessing a new class of cationic aNHC ligands electronically distinct from normal NHCs and aNHCs. These palladium complexes represent the first ex les of transition metal-ligated aNHC complexes featuring a cationic moiety adjacent to the abnormal carbene center. It was anticipated that these design principles could facilitate electron transfer between the imidazolinylidene and the cationic heterocycle, thus reducing the electron density at the abnormal carbene center. However, this case study suggests that greater conformational restrictions that allow for heterocycle coplanarity are necessary to achieve significant electron transfer and enable access to a new class of cationic charge-appended aNHCs with unique electronic properties.
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C002778B
Abstract: Reactions of a dimetallated N,N'-dimethyl substituted porphyrinogen Sm(II) complex with a series of t-butyl substituted heteroalkynes affords a erse range of reactivity. The phosphaalkyne t-BuC[triple bond]P gives a dinuclear Sm(III) P-P reductively coupled complex of (t-BuC=PP=C-t-Bu)(2-) featuring a new mu-eta(2)(1,2-C,P) binding mode. In contrast, the nitrile aza analogue t-BuC[triple bond]N forms Sm(II) adducts that undergo reductive C-C bond cleavage at elevated temperatures to afford a trimeric Sm(III) cyanide (mu-C[triple bond]N(-)) complex. The isomeric isonitrile t-BuN[triple bond]C undergoes the related reductive C-N bond cleavage reactivity at milder temperatures, allowing the trapping of the tert-butyl fragment as a Sm(III) eta(2)-iminoacyl (t-BuC=N-t-Bu)(-) complex.
Publisher: Royal Society of Chemistry (RSC)
Date: 1992
DOI: 10.1039/C39920001423
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6DT01113F
Abstract: The hydroalumination–isomerisation of α- and internal olefins catalysed by bis(imino)pyridine cobalt complexes is investigated.
Publisher: Springer Science and Business Media LLC
Date: 31-10-2019
DOI: 10.1038/S41467-019-12760-Y
Abstract: Systemic sclerosis (SSc) is an autoimmune disease that shows one of the highest mortality rates among rheumatic diseases. We perform a large genome-wide association study (GWAS), and meta-analysis with previous GWASs, in 26,679 in iduals and identify 27 independent genome-wide associated signals, including 13 new risk loci. The novel associations nearly double the number of genome-wide hits reported for SSc thus far. We define 95% credible sets of less than 5 likely causal variants in 12 loci. Additionally, we identify specific SSc subtype-associated signals. Functional analysis of high-priority variants shows the potential function of SSc signals, with the identification of 43 robust target genes through HiChIP. Our results point towards molecular pathways potentially involved in vasculopathy and fibrosis, two main hallmarks in SSc, and highlight the spectrum of critical cell types for the disease. This work supports a better understanding of the genetic basis of SSc and provides directions for future functional experiments.
Publisher: American Chemical Society (ACS)
Date: 23-02-2011
DOI: 10.1021/OM101114C
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3DT32465F
Abstract: A number of analogues of the Mitsui Chemicals ethylene trimerisation system (IV) have been explored, in which one of the donor atoms have been modified. Thus, a series of mono-anionic tridentate phenoxy-imine (3-(t-butyl)-2-(OH)-C6H4C=N(C(CH3)2CH2OMe) 1, 3-(adamantyl)-2-(OH)-C6H4C=N(2'-(2''-(SMe)C6H4)-C6H4) 2, 3-(t-butyl)-2-(OSiMe3)-C6H4C=N(C(CH3)2CH2OMe) 3) or phenoxy-amine (3,5-di(t-butyl)-2-(OH)-C6H4CH2-N(2'-(2''-(OMe)C6H4)-C6H4) 4) ligands have been prepared and reacted with TiCl4 or TiCl4(thf)2 to give the mono-ligand complexes 5-7. The solid state structures of compounds 4-6 have been determined. Complexes 5-7 have been tested for their potential as ethylene oligomerisation olymerisation systems in conjunction with MAO activator and benchmarked against the Mitsui phenoxy-imine trimerisation system IV. While the phenoxy-amine complex 6 shows a propensity for polymer formation, the phenoxy-imine complexes 5 and 7 show somewhat increased formation of short chain LAOs. Complex 5 is selective for 1-butene in the oligomeric fraction, while 7 displays liquid phase selectivity to 1-hexene. As such 7, which is a sulfur substituted analogue of the Mitsui system IV, displays similar characteristics to the parent catalyst. However, its utility is limited by the lower activity and predominant formation of polyethylene.
Publisher: Wiley
Date: 17-01-2019
Abstract: A synthesis of unconjugated (E)-enediynes from allenyl amino alcohols is reported and their gold-catalyzed cascade cycloaromatization to a broad range of enantioenriched substituted isoindolinones has been developed. Experimental and computational studies support the reaction proceeding via a dual-gold σ,π-activation mode, involving a key gold-vinylidene- and allenyl-gold-containing intermediate.
Publisher: IGI Global
Date: 2011
DOI: 10.4018/978-1-61350-062-0.CH003
Abstract: A number of in-class and post-lecture learning strategies are described that have recently been incorporated into the first year chemistry program at the University of Tasmania, Hobart. These methodologies are centered on supporting the various language based challenges that students face in achieving a firm introduction to the discipline. A number of delivery strategies were trialed for in-class activities that overcame institutional specific limitations in access to technologies in an attempt to increase student involvement in lectures and tutorials. Activities included mobile phone-based technologies (and simple overhead transparency/show-of-hand alternatives) for in-class audience surveys, word matching exercises, and chemical songs. The post-lecture approaches also covered a range of delivery platforms, including (i) on-line based quizzes that focused on providing specific, tailored feedback to allow maximal self-reflection on the understanding of key terms and concepts prior to attempting weekly summative assignments where feedback is deliberately kept limited (ii) developing a broader range of weekly assignment questions (beyond conventional multiple choice) to focus on language issues (iii) chemical Sudoku puzzles, and (iv) crossword activities. Evaluations of these approaches are presented.
Publisher: Elsevier BV
Date: 04-2011
Publisher: Wiley
Date: 08-03-2010
Publisher: Elsevier BV
Date: 10-2011
Publisher: Royal Society of Chemistry (RSC)
Date: 1995
DOI: 10.1039/C39950002501
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C0DT01266A
Abstract: A synthetic and structural (X-ray) investigation into the bonding modes of benzoxazole (box) and 2-methylbenzoxazole (Mebox) ligands with halide precursors of Zn and Pd has been undertaken to clarify earlier discrepancies concerning the nature of the bonding mode(s) of the two azoles. In four structurally characterised ex les, all contain the title ligands in a κ(1)N bonding motif. Calculations at the density functional level (DFT) of theory (B3LYP) confirm the ground state stability of this class of coordination for several hypothetical Pd and Zn (gas phase) compounds. The attempt to obtain suitable crystalline material of PdCl(2)(box)(2) (i.e., 5) leads to substantial complex degradation. One minor product of this process has been identified (X-ray) as the diarylformamidinato complex C(26)H(22)N(4)O(4)Pd, presumably formed via a complex combination of the decomposition products of both free box and 5.
Publisher: Royal Society of Chemistry (RSC)
Date: 1992
DOI: 10.1039/C39920001154
Publisher: Wiley
Date: 09-09-2014
Publisher: International Union of Crystallography (IUCr)
Date: 26-01-2007
Publisher: American Chemical Society (ACS)
Date: 26-07-2019
Publisher: Wiley
Date: 19-08-2022
Abstract: Diene‐transmissive hetero‐Diels–Alder sequences involving carbonyl dienophiles are reported for the first time. High enantioselectivities are achieved in the reaction of phenylglyoxal with a broad range of dendralene structures, through the optimization of a Pd 2+ catalyst system. The initial catalyst‐controlled enantioselective oxa‐Diels–Alder (ODA) cycloaddition to a [3]dendralene generates a dihydropyran carrying a semicyclic diene. This participates in a subsequent catalyst or substrate‐controlled Diels–Alder reaction to generate sp 3 ‐rich fused polycyclic systems containing both heterocycles and carbocycles. Computational investigations reveal a concerted asynchronous mechanism. π‐Complexation of a diene C=C bond to Pd 2+ occurs in both the pre‐transition state (TS) complex and in cycloaddition TSs, controlling stereoselectivity. A formal enantioselective [4+2]cycloaddition of a CO 2 dienophile is demonstrated.
Publisher: Royal Society of Chemistry (RSC)
Date: 2002
DOI: 10.1039/C5OB02577J
Abstract: The in situ reduction of ferrocenyl cyclopropylimines to the corresponding amines triggers a facile oxidative ring-opening to yield the formal four-electron oxidation products: N -ferrocenylmethyl β-hydroxyamides.
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/C001109F
Abstract: An unreported product outcome from an intended Sonogashira coupling is presented. The generality of this finding has been demonstrated by screening of a range of pre-catalysts. Mechanistic studies are consistent with the tetra-aryl benzene product forming by interception of the aryl halide oxidative addition intermediate by repeated acetylene insertion.
Publisher: Wiley
Date: 13-03-2020
Abstract: The most pressing challenges for light‐driven hydrogel actuators include reliance on UV light, slow response, poor mechanical properties, and limited functionalities. Now, a supramolecular design strategy is used to address these issues. Key is the use of a benzylimine‐functionalized anthracene group, which red‐shifts the absorption into the visible region and also stabilizes the supramolecular network through π–π interactions. Acid–ether hydrogen bonds are incorporated for energy dissipation under mechanical deformation and maintaining hydrophilicity of the network. This double‐crosslinked supramolecular hydrogel developed via a simple synthesis exhibits a unique combination of high strength, rapid self‐healing, and fast visible‐light‐driven shape morphing both in the wet and dry state. As all of the interactions are dynamic, the design enables the structures to be recycled and reprogrammed into different 3D objects.
Publisher: American Chemical Society (ACS)
Date: 19-08-2020
DOI: 10.26434/CHEMRXIV.12812000
Abstract: Despite their apparent similarity, framework materials based on tetraphenylmethane and tetraphenylsilane building blocks often have quite different structures and topologies. Herein, we describe a new silicon tetraamidinium compound and use it to prepare crystalline hydrogen bonded frameworks with carboxylate anions in water. The silicon-containing frameworks are compared with those prepared from the analogous carbon tetraamidinium: when biphenyldicarboxylate or tetrakis(4-carboxyphenyl)methane anions were used similar channel-containing networks are observed for both the silicon and carbon tetraamidinium. When terephthalate or bicarbonate anions were used, different products form. Insights into possible reasons for the different products are provided by a survey of the Cambridge Structural Database and quantum chemical calculations, both of which indicate that, contrary to expectations, tetraphenylsilane derivatives have less geometrical flexibility than tetraphenylmethane derivatives, i.e. they are less able to distort away from ideal tetrahedral bond angles. / / /
Publisher: Royal Society of Chemistry (RSC)
Date: 2005
DOI: 10.1039/B500198F
Abstract: The first structurally authenticated 4-azapentalenyl complexes are reported, along with DFT studies, that reveal tendencies for their cyclopentadienyl isostructural nature and an ability to exhibit binding modes of varying hapticity.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3CC41209A
Abstract: Herein we describe a CuAAC "click" methodology for exo-functionalisation of Pd2L4 metallosupramolecular architectures. The potentially coordinating 1,2,3-triazole does not affect formation of the desired discrete complexes, nor does this external functional decoration affect the cisplatin-binding ability of the interior cavity of the assembly.
Publisher: ARKAT USA, Inc.
Date: 26-04-2013
Publisher: Wiley
Date: 15-12-2020
Publisher: Elsevier BV
Date: 2010
Publisher: American Chemical Society (ACS)
Date: 12-2016
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC02244E
Abstract: The results of a proof-of-concept study demonstrate for the first time that pulsed LED irradiation enhances the rate of product formation and the yield of a visible light-mediated photoredox-catalysed reaction.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3SC52072B
Abstract: Actinide complexes of a small-cavity, dipyrrolide macrocycle exhibit unusual bent metallocene-type binding, or bis(arene)-type binding, or both at once in a di-uranium adduct.
Publisher: American Chemical Society (ACS)
Date: 21-01-2015
DOI: 10.1021/JP510827H
Abstract: Conjecture existed as to the molecular structure of the crystalline organic peroxide reaction product derived from the acidified aqueous mixture of urea, formaldehyde, and hydrogen peroxide. This study used X-ray crystal structure determination to unequivocally define the reaction product as the 14-membered ring structure tetramethylene diperoxide dicarbamide (TMDD). Crystals of TMDD belong to the monoclinic space group Pc, a = 4.587(4), b = 16.080(2), c = 6.690(5) Å, β = 107.44(5)°. The crystal contains one crystallographically independent molecule with approximate Cs symmetry. Intramolecular π-stacking of the carbonyl groups is a feature, while intermolecular H-bonding between the N-H and C═O functionalities affords linear polymeric strands that is associated with the extremely fine needle crystal morphology that necessitated synchrotron radiation for the structure determination. Sensitiveness testing examining susceptibility to initiate due to heat, impact, friction, and electrostatic stimuli was conducted to gauge the hazards associated with the material. It was revealed to be a primary explosive, particularly susceptible to impact initiation.
Publisher: MDPI AG
Date: 04-12-2018
DOI: 10.3390/CATAL8120620
Abstract: Ongoing research exploring the chemistry of N-heterocyclic carbenes (NHCs) has led to the development and discovery of new NHC subclasses that deviate beyond Arduengo’s prototypical N,N′-disubstituted imidazol-2-ylidene-based structures. These systems continue to enable and extend the fundamental role of NHC ligands in synthesis and catalysis. In this regard, the advent of protic NHCs has garnered particular interest. This derives in part from their applications to the selective preparation of unique molecular scaffolds and their unprecedented bifunctional reactivity, which can be exploited in transition metal-catalyzed processes. In comparison, the synthetic applications of closely related anionic naked NHCs remain rather underexplored. With this in mind, this review highlights the interesting fundamental properties of non-classical anionic naked NHCs, and focuses on their emerging applications in synthesis and catalysis.
Publisher: Wiley
Date: 23-03-2022
Abstract: An isostructural series of heavy Group 14 E(I) radical anions (Ge, Sn, Pb), stabilized by a bulky xanthene‐based diamido ligand are reported. The radical anions were synthesised by the one‐electron reduction of their corresponding E(II) precursor complexes with sodium naphthalenide in THF, yielding the radical anions as charge‐separated sodium salts. The series of main group radicals have been comprehensively characterized by EPR spectroscopy, X‐ray crystallography and DFT analysis, which reveal that in all cases, the spin density of the unpaired electron almost exclusively resides in a p ‐orbital of π symmetry located on the Group 14 center.
Publisher: Elsevier BV
Date: 2005
Publisher: American Chemical Society (ACS)
Date: 04-01-2017
Publisher: Wiley
Date: 21-12-2019
Publisher: CSIRO Publishing
Date: 2011
DOI: 10.1071/CH11095
Abstract: Synchrotron data have been used to determine the structures of the yellow polymorph of dichlorido(2,2′-bipyridine)platinum(ii) (1), and diiodido(2,2′-bipyridine)palladium(ii) (2), allowing a detailed comparison of the crystal chemistry of [MX2(bipy)] (M = Pd, Pt X = Cl, Br, I), which exhibit polymorphism involving nine structures distributed over five space groups. Complex 1 crystallizes in space group Pbca (a = 18.2540(7), b = 15.6970(7), c = 7.3560(6) Å), and 2 in space group C2/c (a = 17.149(1), b = 9.8050(8), c = 7.548(1) Å, β = 110.72(1) °).
Publisher: MDPI AG
Date: 02-2010
DOI: 10.3390/MA3020841
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3DT32895C
Abstract: N,N'-Asymmetrically substituted, methylene-linked bis(imidazol-2-ylidene) complexes have been prepared subsequent to a selective synthesis of the bis(imidazolium) salt precursors involving the quarternisation of N-alkyl and -aryl imidazoles with N-halomethyl imidazolium salts. The adaptability of the ligand precursor synthesis is illustrated through access to the N-Me/N'-Mes and N-Mes/N'-2,6-(i-Pr)2Ph systems, leading to the Pd(II) complexes [{(MeIm)(MesIm)CH2}Pd(L)2](n+), L = Cl/I (n = 0) and NCMe (n = 2), and [{(MesIm)[2,6-(i-Pr)2PhIm]CH2}Pd(L)2], L = Cl/I. The dicationic hybrid N,N'-alkyl/aryl complex was inactive in the copolymerisation of ethylene/carbon monoxide, displaying reactivity akin to N,N'-dialkyl analogues.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9SC03215K
Abstract: The first reported catalytic reactivity of 5-allenyloxazolidinones is the tightly controlled, ergent synthesis of chiral 1,3-dienes or 5-vinyloxazolidinones under Pd(0) catalysis.
Publisher: American Chemical Society (ACS)
Date: 12-06-2019
DOI: 10.1021/ACS.ORGLETT.9B01580
Abstract: Aminobenzaldehydes bearing a pendant 3,5-dinitrophenyl group react thermally with N-substituted α-amino acids to form unprecedented benzoazepine-fused isoindolines. The reaction proceeds via a dearomatization/rearomatization sequence involving an intramolecular (3 + 2)-cycloaddition between the in situ formed azomethine ylide and the dinitroarene. Various glycine derivatives are tolerated as well as branched substrates based on cyclic, α-mono-, and α,α-disubstituted amino acids, giving single diastereomers in many cases. The method is scalable and gives products with a nitro group ready for further manipulation.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4FD00182F
Abstract: We use density-functional theory molecular dynamics (DFT-MD) simulations to determine the hydride transfer coordinate between palladium centres of the crystallographically observed terminal hydride locations, Pd–Pd–H, originally postulated for the solution dynamics of the complex bis-NHC dipalladium hydride [{(MesIm) 2 CH 2 } 2 Pd 2 H][PF 6 ], and then calculate the free-energy along this coordinate. We estimate the transfer barrier-height to be about 20 kcal mol −1 with a hydride transfer rate in the order of seconds at room temperature. We validate our DFT-MD modelling using inelastic neutron scattering which reveals anharmonicity of the hydride environment that is so pronounced that there is complete failure of the harmonic model for the hydride ligand. The simulations are extended to high temperature to bring the H-transfer to a rate that is accessible to the simulation technique.
Publisher: Elsevier BV
Date: 11-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 11-12-2003
DOI: 10.1039/B210600K
Publisher: American Chemical Society (ACS)
Date: 07-05-2009
DOI: 10.1021/JA902799U
Abstract: A study of the reaction of PtMe(2)(bipy) with IPh(C[triple bond]CSiMe(3))(OTf) at low temperature in acetone, leading to detection of the Pt-Pt-bonded cation [Pt(2)Me(4)(C[triple bond]CSiMe(3))(bipy)(2)](+), an intermediate in the oxidation of Pt(II) to Pt(IV), is reported. The cation is assessed as Pt(III)-Pt(III) Pt(IV)-Pt(II), and at the other extreme may be regarded as a cationic alkynylplatinum(IV) center, "[Pt(IV)Me(2)(C[triple bond]CSiMe(3))(bipy)](+)", stabilized by "Pt(II)Me(2)(bipy)" as a donor ligand. The detection and isolation of the [Pt(2)Me(4)(C[triple bond]CSiMe(3))(bipy)(2)](+) cation provides a number of insights into the mechanisms of oxidation reactions.
Publisher: American Chemical Society (ACS)
Date: 04-12-2017
Abstract: A trans-diastereoselective Pd-catalyzed dearomative [3 + 2] cycloaddition between vinylcyclopropane dicarboxylates and 3-nitroindoles has been developed. The reaction provides densely functionalized cyclopenta[b]indolines with versatile vinyl and nitro-groups. The addition of a halide additive was found to be critical for the diastereoselectivity of the reaction, which is proposed to be a result of a rapid π-σ-π interconversion between the intermediates allowing for Curtin-Hammett control. A switch in diastereoselectivity to afford products with the vinyl and nitro groups cis to each other is observed with a 4-substituted 3-nitroindole.
Publisher: Hindawi Limited
Date: 24-06-2019
DOI: 10.1111/ANE.13132
Abstract: Modifiable lifestyle factors are implicated in multiple sclerosis (MS) symptoms but their role in mood is unclear. This study aimed to investigate associations between lifestyle and depression and anxiety in Australian participants with MS. Self-reported data from the Australian Multiple Sclerosis Longitudinal Study included the Hospital Anxiety and Depression Scale (HADS) and lifestyle measurements from 1500 participants. SNAP score (range 0-5) was the sum of non-smoking, sufficient fruit/vegetable intake, non-hazardous alcohol consumption, sufficient physical activity and healthy BMI. Analyses by log-binomial and linear regression were adjusted for confounding. Symptoms of depression and anxiety were prevalent in 27% and 40%, respectively 20% had both. Mean SNAP score was 2.7/5 only 3% met all healthy lifestyle recommendations. Only 10% reported adequate fruit/vegetable intake, and 22% reported a combination of unhealthy BMI, inadequate physical activity and inadequate nutrition. A healthier SNAP score was associated with lower depression prevalence (adjusted prevalence ratio 0.83 [95% CI 0.75, 0.92] per unit increase) and depression severity (adjusted β-0.44 [95% CI -0.64, -0.24]), but not with anxiety. Modifiable lifestyle factors are associated with lower frequency and severity of depression, but not anxiety, in Australian people with multiple sclerosis. The associations between a healthier SNAP score and lower depression are likely bi-directional. SNAP risk factor prevalence and co-occurrence, especially inadequate nutrition and low physical activity, were high among Australians with MS.
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4CY00457D
Abstract: Selected phosphine-based ligands plus chromium have been found to be promising candidates for MAO-free trimerisation and tetramerisation of ethylene.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC01554D
Abstract: The potassium aluminyl K[Al(NON Dipp )] promotes the reductive homologation of CO to afford the [C 4 O 4 ] 4− (2 isomers) and [C 5 O 5 ] 5− ligands.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C0MD00211A
Publisher: Cold Spring Harbor Laboratory
Date: 24-07-2019
DOI: 10.1101/712398
Abstract: The electrocardiographic PR interval reflects atrioventricular conduction, and is associated with conduction abnormalities, pacemaker implantation, atrial fibrillation (AF), and cardiovascular mortality 1,2 . We performed multi-ancestry (N=293,051) and European only (N=271,570) genome-wide association (GWAS) meta-analyses for the PR interval, discovering 210 loci of which 149 are novel. Variants at all loci nearly doubled the percentage of heritability explained, from 33.5% to 62.6%. We observed enrichment for genes involved in cardiac muscle development/contraction and the cytoskeleton highlighting key regulation processes for atrioventricular conduction. Additionally, 19 novel loci harbour genes underlying inherited monogenic heart diseases suggesting the role of these genes in cardiovascular pathology in the general population. We showed that polygenic predisposition to PR interval duration is an endophenotype for cardiovascular disease risk, including distal conduction disease, AF, atrioventricular pre-excitation, non-ischemic cardiomyopathy, and coronary heart disease. These findings advance our understanding of the polygenic basis of cardiac conduction, and the genetic relationship between PR interval duration and cardiovascular disease.
Publisher: MDPI AG
Date: 30-06-2018
DOI: 10.3390/CATAL8070268
Publisher: Royal Society of Chemistry (RSC)
Date: 2006
DOI: 10.1039/B611784H
Abstract: A macrocyclic organosamarium(II) complex has been shown to provide the first ex le of the reductive disproportionation of carbon dioxide, giving a bimetallic carbonate complex and carbon monoxide in a facile reaction under ambient conditions.
Publisher: American Chemical Society (ACS)
Date: 02-2005
DOI: 10.1021/OM0490233
Publisher: Wiley
Date: 05-2004
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9CC06707H
Abstract: A 3D hydrogen bonded organic framework was assembled in water from tetraamidinium cations and antielectrostatically hydrogen bonded bicarbonate dimers.
Publisher: Wiley
Date: 11-2013
Abstract: Language impairment (LI) in the preschool years is known to vary over time. Stability in the diagnosis of LI may be influenced by children’s in idual variability, the measurement error of commonly used assessment instruments and the cut-points used to define impairment. To investigate the agreement between two different age-based versions of a language assessment instrument and the stability of the classification of LI using the two measures over a 12-month period. A total of 945 participants completed the Clinical Evaluation of Language Fundamentals(CELF—Preschool 2 or 4th Edn) at 4 and 5 years of age. Agreement and stability were analysed using Bland–Altman plots, correlation and odds ratios. Sensitivity and specificity were calculated for two thresholds of the CELF-P2 using the diagnostic category on the child’s subsequent CELF-4. For all CELF scores, mean differences for the cohort between 4 and 5 years were within 1.5 scale score units. In contrast, at the in idual level variability was found across the range of scores and was of a greater magnitude than previously reported. Stability in LI classification was low, with 36% of 5-year-olds with LI (defined as a standard score below –1.25) classified as typical at 4 years, even though odds ratios calculated from classifications at the two time points suggested that 4-year-olds with LI had 23 times greater odds than their typical peers to receive a diagnosis of LI at 5 years. The CELF-P2 did not demonstrate adequate levels of diagnostic accuracy for LI at 5 years: sensitivity of 64% and specificity of 92.9%. Substantial variability across the entire range of possible CELF scores was observed in this community cohort between the ages of 4 and 5 years. The stability of LI classification was lower than that reported in previous research conducted primarily on smaller clinical cohorts. The current study’s results suggest that the variability observed in developmental language pathways is the result of a combination of limitations in measurement instruments, in idual children’s abilities and the arbitrary nature of the boundaries defining LI.
Publisher: Elsevier BV
Date: 12-2010
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1OB05665D
Abstract: Thirteen enantiopure paddlewheel-shaped dirhodium(II) tetrakiscarboxylate complexes have been checked for their efficiency in the dirhodium method (differentiation of enantiomers by NMR spectroscopy) six of them are new. Their diastereomeric dispersion effects were studied and compared via so-called key numbers KN. Adducts of each complex were tested with five different test ligands representing all relevant donor properties from strong (phosphane) to very weak (ether). Only one of them, the dirhodium complex with four axial (S)-N-2,3-naphthalenedicarboxyl-tert-leucinate groups (N23tL), showed results significantly better for all ligands than the conventional complex Rh* [Rh(II)(2)[(R)-(+)-MTPA](4) MTPA = methoxytrifluoromethylphenylacetate]. On the basis of (1)H{(1)H} NOE spectroscopy and X-ray diffraction, a combination of favourable anisotropic group orientation and conformational flexibility is held responsible for the high efficiency of N23tL in enantiodifferentiation. Both complexes, Rh* and N23tL, are recommended as chiral auxiliaries for the dirhodium experiment.
Publisher: Elsevier BV
Date: 2012
Publisher: Elsevier BV
Date: 05-1993
Publisher: American Chemical Society (ACS)
Date: 30-08-2019
DOI: 10.26434/CHEMRXIV.9746195
Abstract: Crystalline 3D hydrogen bonded frameworks are assembled in water from tetrahedral tetraamidinium cations and antielectrostatically hydrogen bonded bicarbonate dimers. The framework forms in water, and represents a clear demonstration of the potency of these anti-Coulombic hydrogen bonds. Gentle heating of the framework (50 °C) releases CO2 and water to give the neutral tetraamidine compound.
Publisher: Wiley
Date: 03-2008
Publisher: Wiley
Date: 19-08-2022
Abstract: Diene‐transmissive hetero‐Diels–Alder sequences involving carbonyl dienophiles are reported for the first time. High enantioselectivities are achieved in the reaction of phenylglyoxal with a broad range of dendralene structures, through the optimization of a Pd 2+ catalyst system. The initial catalyst‐controlled enantioselective oxa‐Diels–Alder (ODA) cycloaddition to a [3]dendralene generates a dihydropyran carrying a semicyclic diene. This participates in a subsequent catalyst or substrate‐controlled Diels–Alder reaction to generate sp 3 ‐rich fused polycyclic systems containing both heterocycles and carbocycles. Computational investigations reveal a concerted asynchronous mechanism. π‐Complexation of a diene C=C bond to Pd 2+ occurs in both the pre‐transition state (TS) complex and in cycloaddition TSs, controlling stereoselectivity. A formal enantioselective [4+2]cycloaddition of a CO 2 dienophile is demonstrated.
Publisher: CSIRO Publishing
Date: 2023
DOI: 10.1071/CH23130
Publisher: American Chemical Society (ACS)
Date: 04-05-2010
DOI: 10.1021/AC100417H
Abstract: The present study describes a preparative gas chromatographic (GC) approach employed to study a series of products arising from reaction of phenylacetylene with para-substituted aryl-iodides under Sonogashira catalysis conditions. GC analysis resolves the isomers from each reaction however, it cannot provide structural details (their MS data are virtually identical). Since classical liquid chromatography cannot resolve the isomers, preparative-scale GC is the only practical approach to provide further spectroscopic characterization of the isomers. The products are well separated by GC so a single thick-film capillary column is adequate for this case, with operation up to approximately +300 degrees C. By collection of 50+ repeat injections, sufficient material could be isolated for (1)H NMR spectral analysis of the isomers, and for one isomer (isomer I) of a number of analogous related catalytic reaction mixtures, X-ray crystal structure determination enabled complete structural elucidation (absolute configuration) of the substitution pattern of the structure of this isomer. This confirmed isomer I to be the 2-para-aryl-substituted 1,3,5-triphenylbenzene product in all cases. (1)H NMR spectra of isomer I products generally had similar patterns but differed markedly from the second major isomer product (isomer II).
Publisher: Royal Society of Chemistry (RSC)
Date: 1995
DOI: 10.1039/C39950001457
Publisher: American Chemical Society (ACS)
Date: 30-08-2019
DOI: 10.26434/CHEMRXIV.9746195.V1
Abstract: Crystalline 3D hydrogen bonded frameworks are assembled in water from tetrahedral tetraamidinium cations and antielectrostatically hydrogen bonded bicarbonate dimers. The framework forms in water, and represents a clear demonstration of the potency of these anti-Coulombic hydrogen bonds. Gentle heating of the framework (50 °C) releases CO2 and water to give the neutral tetraamidine compound.
Publisher: International Union of Crystallography (IUCr)
Date: 10-01-2007
Publisher: Wiley
Date: 23-03-2022
Abstract: An isostructural series of heavy Group 14 E(I) radical anions (Ge, Sn, Pb), stabilized by a bulky xanthene‐based diamido ligand are reported. The radical anions were synthesised by the one‐electron reduction of their corresponding E(II) precursor complexes with sodium naphthalenide in THF, yielding the radical anions as charge‐separated sodium salts. The series of main group radicals have been comprehensively characterized by EPR spectroscopy, X‐ray crystallography and DFT analysis, which reveal that in all cases, the spin density of the unpaired electron almost exclusively resides in a p ‐orbital of π symmetry located on the Group 14 center.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5DT00955C
Abstract: In idual steps of the aluminium-mediated contrathermodynamic isomerisation of internal olefins to α-olefins are studied.
Publisher: Wiley
Date: 02-02-2016
Abstract: A novel approach to the design of dirhodium(II) tetracarboxylates derived from (S)-amino acid ligands is reported. The approach is founded on tailoring the steric influences of the overall catalyst structure by reducing the local symmetry of the ligand's N-heterocyclic tether. The application of the new approach has led to the uncovering of [Rh
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC01510F
Abstract: Formation of valuable spiroheterocycles with multiple contiguous stereogenic centres from palladium-catalysed enantioselective (3 + 2) cycloaddition reactions of sulfamidate-derived azadienes and vinylcyclopropanes.
Publisher: Elsevier BV
Date: 06-2013
DOI: 10.1016/J.ORALONCOLOGY.2013.01.006
Abstract: Novel therapies are required for patients with recurrent or metastatic oral tongue squamous cell carcinoma (OTSCC). Fibroblast Growth Factor Receptor 1 (FGFR1) lification frequently occurs in squamous cell carcinoma of the lung and represents a novel druggable therapeutic target in this and other malignancies. This study examined the frequency and clinical associations of FGFR1 lification in OTSCC. The frequency of FGFR1 lification determined by fluorescence in situ hybridization was evaluated in a cohort of 123 OTSCC patients. Associations of FGFR1 lification with clinical characteristics and outcome were determined. FGFR1 gene lification was present in 9.3% (10/107) of cases and was significantly associated with smoking status (P = 0.03). FGFR1 lification was seen more commonly in males (9/10 lified cases male, P = 0.16) and there were no associations with age, stage, T stage, nodal status, alcohol history or performance status (all P>0.05). Outcome was not significantly different between FGFR1 lified and non- lified patients. Copy number variations of the FGFR1 gene occur in a subset of OTSCC with approximately 10% of cases showing lification of the gene. FGFR1 lification may represent a therapeutic target in OTSCC.
Publisher: Elsevier BV
Date: 09-2009
No related grants have been discovered for Michael Gardiner.