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    ABSTRACT: Well-defined alkyl chain side group polymer brushes have been tethered onto high surface area macroporous pulsed plasmachemical emulsion-templated poly(vinylbenzyl chloride) initiator layers (typically 600-700m(2)g(-1)) using atom transfer radical polymerisation (ATRP). Immobilisation of phospholipids onto these bioactive surfaces is found to occur through interdigitation, and the efficacy of lipid binding is governed by the alkyl side group chain length of the polymer brushes.
    Journal of Colloid and Interface Science 01/2014; 421:44–48.
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    ABSTRACT: Dehydrobutyrine is an amino acid that is present in a range of peptide natural products. Reaction of pentafluoropyridine with threonine and subsequent E1cb-type elimination allowed the preparation of novel dehydrobutyrine-containing amino acids under mild conditions.Figure optionsDownload full-size imageDownload as PowerPoint slide
    Tetrahedron. 01/2014; 70(31):4661–4667.
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    Tetrahedron 01/2014; 70(34):5182–5189.
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    ABSTRACT: Seven oxyselenide materials have been synthesised with composition A4O4TiSe4 (A=Sm, Gd–Er, Y) via solid state reactions of A2O3, TiSe2 and Se at 900 °C. They are all isostructural with Gd4O4TiSe4. Structures have been refined from powder X-ray diffraction data and have monoclinic C2/m symmetry with unit cell parameters of a≈15.7 Å, b≈3.75 Å, c≈9.65 Å and β≈117.5°. They contain infinite ribbons of edge-sharing A4O and A3TiO tetrahedra 4 units wide, which are linked by chains of TiSe4O2 edge-sharing octahedra. Compositions A=Gd–Ho, Y are semiconductors with conductivities 1–3 Sm−1 at 300 K, with electronic band gaps of between 0.25 and 0.37 eV. Magnetic susceptibility is reported from 1.8 K to 300 K for compositions A=Gd–Ho. Rare earth moments appear to order antiferromagnetically at low temperatures with Gd and Tb showing evidence of ferromagnetism due to spin canting over a narrow temperature range close to TN.
    ChemInform 01/2014; 210(1):188–194.
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    ABSTRACT: Blending different low molecular weight gelators (LMWGs) provides a convenient route to tune the properties of a gel and incorporate functionalities such as fluorescence. Blending a series of gelators having a common bis-urea motif, and functionalised with different amino acid-derived end-groups and differing length alkylene spacers is reported. Fluorescent gelators incorporating 1- and 2-pyrenyl moieties provide a probe of the mixed systems alongside structural and morphological data from powder diffraction and electron microscopy. Characterisation of the individual gelators reveals that although the expected α-urea tape motif is preserved, there is considerable variation in the gelation properties, molecular packing, fibre morphology and rheological behaviour. Mixing of the gelators revealed examples in which: 1) the gels formed separate, orthogonal networks maintaining their own packing and morphology, 2) the gels blended together into a single network, either adopting the packing and morphology of one gelator, or 3) a new structure not seen for either of the gelators individually was created. The strong binding of the urea functionalities to anions was exploited as a means of breaking down the gel structure, and the use of fluorescent gel blends provides new insights into anion-mediated gel dissolution.
    Chemistry 12/2013;
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    ABSTRACT: Tuberculosis remains the second only to HIV as the leading cause of death by infectious disease worldwide, and was responsible for 1.4 million deaths globally in 2011. One of the essential drugs of the second-line antitubercular regimen is the prodrug ethionamide, introduced in the 1960s. Ethionamide is primarily used in cases of multi-drug resistant (MDR) and extensively drug resistant (XDR) TB due to severe adverse side effects. As a prodrug, ethionamide is bioactivated by EthA, a mono-oxygenase whose activity is repressed by EthR, a member of the TetR family of regulators. Previous studies have established that inhibition of EthR improves ethionamide potency. We report here the crystal structures of three EthR inhibitors at 0.8 Å resolution (3-oxo-3-{4-[3-(thiophen-2-yl)-1,2,4-oxadiazol-5-yl]piperidin-1-yl}propanenitrile (BDM31343), 4,4,4-trifluoro-1-{4-[3-(6-methoxy-1,3-benzothiazol-2-yl)-1,2,4-oxadiazol-5-yl]piperidin-1-yl}butanone (BDM41325) and 5,5,5-trifluoro-1-{4-[3-(4-methanesulfonylphenyl)-1,2,4-oxadiazol-5-yl]piperidin-1-yl}pentanone (BDM41907)), and the docking studies undertaken to investigate possible binding modes. The results revealed two distinct orientations of the three compounds in the binding channel, a direct consequence of the promiscuous nature of the largely lipophilic binding site.
    Acta Crystallographica Section C Crystal Structure Communications 11/2013; 69(Pt 11):1243-50.
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    ABSTRACT: We show theoretically that ultracold hydrogen atoms have very favorable properties for sympathetic cooling of molecules to microkelvin temperatures. We calculate the potential energy surfaces for spin-polarized interactions of H atoms with the prototype molecules NH(^{3}Σ^{-}) and OH(^{2}Π) and show that they are shallow (50 to 80 cm^{-1}) and only weakly anisotropic. We carry out quantum collision calculations on H+NH and H+OH and show that the ratio of elastic to inelastic cross sections is high enough to allow sympathetic cooling from temperatures well over 1 K for NH and around 250 mK for OH.
    Physical Review Letters 11/2013; 111(20):203004.
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    ABSTRACT: The photoelectron imaging of the indigo carmine dianion is used to demonstrate the effects of resonance excitation, pulse duration and pulse intensity on the photoelectron spectra and angular distributions of a dianion. Excitation of the S1 state leads to an aligned distribution of excited state dianions. The photoelectron angular distribution following subsequent photodetachment within a femtosecond laser pulse is primarily determined by the repulsive Coulomb barrier. Extending the timescale for photodetachment to nanoseconds leads to dramatic changes in both the spectral and angular distributions. These observations are explained in terms of statistical detachment of electrons, either from the monoanion, or from the ground state of the dianion following a number of photon cycles through the S1 ← S0 transition. At high intensity, new electron emission channels open up, leading to emission below the repulsive Coulomb barrier. This has been assigned to strong-field induced detachment and the effect of an electric field on the Coulomb barrier is discussed in terms of the photoelectron spectra and angular distributions.
    Physical Chemistry Chemical Physics 10/2013;
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    ABSTRACT: Atomized spray plasma deposition (ASPD) using a precursor mixture of 2-hydroxyethyl methacrylate and methacryloyl-functionalized 15 nm silica nanoparticles leads to the formation of poly(2-hydroxyethyl methacrylate)-silica nanocomposite layers. The direct application of these coatings to overlapping glass-glass joints gives rise to excellent in situ adhesion reaching 84 MPa shear bond strength and 6 GPa shear modulus prior to the onset of adherent (bulk glass) failure. This significant enhancement in interfacial adhesion arises due to the silica nanoparticle surface methacryloyl groups enhancing cross-linking throughout the nanocomposite layer.
    ACS Applied Materials & Interfaces 09/2013;
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    ABSTRACT: Mono-C-substitution of the 1,4,7-triazacyclononane ring induces formation of single enantiomers of Eu(iii) complexes with nonadentate N6O3 ligands. The absolute configuration of each complex is determined by the stereogenicity of the C-substituent, revealed by comparison of the sign and sequence of CPL transitions for a series of complexes.
    Dalton Transactions 09/2013;
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