M. J. Rosseinsky

University of Liverpool, Liverpool, England, United Kingdom

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Publications (414)2123.05 Total impact

  • Solid State Sciences 11/2014; · 1.67 Impact Factor
  • Christophe Didier, John Claridge, Matthew Rosseinsky
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    ABSTRACT: The title compound is prepared by solid state reaction of stoichiometric mixtures of BaCO3, Ga2O3, and In2O3 (alumina boat, 12 h at either 1100, 1200, or 1300 °C under ambient air) and characterized by powder XRD, time-of-flight neutron diffraction, and impedance measurements.
    ChemInform 10/2014; 45(41).
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    Christophe Didier, John Claridge, Matthew Rosseinsky
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    ABSTRACT: In/Ga cation ordering occurs only for the x=12 composition in brownmillerite Ba2(In1−xGax)2O5. The increased ordering results in an anomalously higher disordering transition temperature to the cubic perovskite.Figure optionsDownload full-size imageDownload as PowerPoint slide
    Journal of Solid State Chemistry 10/2014; 218:38–43. · 2.04 Impact Factor
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    ABSTRACT: Development of heterogeneous catalysts for complex reactions such as Fischer-Tropsch synthesis of fuels is hampered by difficult reaction conditions, slow characterisation techniques such as chemisorption and temperature-programmed reduction and the need for long term stability. High-throughput (HT) methods may help, but their use has until now focussed on bespoke micro-reactors for direct measurements of activity and selectivity. These are specific to individual reactions and do not provide more fundamental information on the materials. Here we report using simpler HT characterisation techniques (XRD and TGA) along with ageing under Fischer-Tropsch reaction conditions to provide information analogous to metal surface area, degree of reduction and thousands of hours of stability testing time for hundreds of samples per month. The use of this method allowed the identification of a series of highly stable, high surface area catalysts promoted by Mg and Ru. In an advance over traditional multichannel HT reactors, the chemical and structural information we obtain on the materials allows us to identify the structural effects of the promoters and their effects on the modes of deactivation observed.
    Chemical Science 10/2014; · 8.31 Impact Factor
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    ABSTRACT: The reaction of NiII with a tetra-benzoate pyrene ligand produces a 3D porous framework based on infinite 1D NiII chains. The NiII–O connectivity and the formation of a hydroxo-bridge (μ3-OH) responsible for the connection of the central NiII atoms within the 1D NiII–(μ3-OH)2–NiII chains can be straightforwardly compared with the TiIV–O–TiIV connectivity seen in TiO2. The arrangement of the TBAPy ligand around the 1D rutile-based chains leads in the generation of a porous framework with two distinct types of pores; based on the chemistries of these two types of pores, one can be labelled as hydrophobic and the other as hydrophilic. The use of different activation methods results in the generation of either a porous framework free of guest molecules or a completely solvent-free material, in which the terminal H2O molecules bound to NiII were removed, leading thus to a framework with open NiII sites. CO2 isotherms collected on both frameworks at 195 K and one barshowed type I isotherms characteristic of microporous materials (BET surface areas for: guest-free framework: 257(3) m2·g–1; solvent-free framework: 362(2) m2·g–1). The affinity of both networks at zero coverage for both CO2 and CH4 was found to be greater when the unsaturated NiII sites are available within the void space.
    Zeitschrift für anorganische Chemie 08/2014; · 1.16 Impact Factor
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    ABSTRACT: Heteroepitaxial growth of BaSnO3 and Ba1−xLaxSnO3 (x = 7%) lanthanum doped barium stannate thin films on different perovskite single crystal (SrTiO3 (001) and SmScO3 (110)) substrates has been achieved by pulsed laser deposition under optimized deposition conditions. X-ray diffraction measurements indicate that the films on either of these substrates are relaxed due to the large mismatch and present a high degree of crystallinity with narrow rocking curves and smooth surface morphology while analytical quantification by proton induced X-ray emission confirms the stoichiometric La transfer from a polyphasic target, producing films with measured La contents above the bulk solubility limit. The films show degenerate semiconducting behavior on both substrates, with the observed room temperature resistivities, Hall mobilities, and carrier concentrations of 4.4 mΩ cm, 10.11 cm2 V−1 s−1, and 1.38 × 1020 cm−3 on SmScO3 and 7.8 mΩ cm, 5.8 cm2 V−1 s−1, and 1.36 × 1020 cm−3 on SrTiO3 ruling out any extrinsic contribution from the substrate. The superior electrical properties observed on the SmScO3 substrate are attributed to reduction in dislocation density from the lower lattice mismatch.
    Applied Physics Letters 08/2014; 105(025104). · 3.52 Impact Factor
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    ABSTRACT: Oligodendrocyte precursor cells (OPCs) have shown high promise as a transplant population to promote regeneration in the central nervous system, specifically, for the production of myelin – the protective sheath around nerve fibers. While clinical trials for these cells have commenced in some areas, there are currently key barriers to the translation of neural cell therapies. These include the ability to (a) image transplant populations in vivo; (b) genetically engineer transplant cells to augment their repair potential; and (c) safely target cells to sites of pathology. Here, we review the evidence that magnetic nanoparticles (MNPs) are a 'multifunctional nanoplatform' that can aid in safely addressing these translational challenges in neural cell/OPC therapy: by facilitating real-time and post-mortem assessment of transplant cell biodistribution, and biomolecule delivery to transplant cells, as well as non-invasive 'magnetic cell targeting' to injury sites by application of high gradient fields. We identify key issues relating to the standardization and reporting of physicochemical and biological data in the field; we consider that it will be essential to systematically address these issues in order to fully evaluate the utility of the MNP platform for neural cell transplantation, and to develop efficacious neurocompatible particles for translational applications.
    Molecular and Cellular Therapies. 07/2014; 2:23.
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    ABSTRACT: A solution chemistry synthetic route yields Cs3C60 with the face-centred cubic structure. The described method uses well-established Schlenk techniques and THF as a solvent. The controlled addition of an organo-metallic salt reducing agent prevents the formation of C604- salts. The final product can be precipitated from the solution using hexane as an anti-solvent.
    Faraday Discussions 07/2014; · 3.82 Impact Factor
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    ABSTRACT: The Extended Module Materials Assembly computational method for structure solution and prediction has been implemented for close-packed lattices. Exploring the family of B-site deficient materials in hexagonal perovskite barium cobalt niobates, it is found that the EMMA procedure returns the experimental structures as the most stable for the known compositions of Ba3CoNb2O9, Ba5Nb4O15 and Ba8CoNb6O24. The unknown compositions Ba11Co2Nb8O33 and Ba13CoNb10O39, having longer stacking sequences, are predicted to form as intergrowths of Ba3CoNb2O9 and Ba5Nb4O15, and are found to have similar stability to pure Ba3CoNb2O9 and Ba5Nb4O15, indicating that it is likely they can be synthesised.
    Physical Chemistry Chemical Physics 05/2014; · 4.20 Impact Factor
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    ABSTRACT: Heteroepitaxial growth of BaSnO$_3$ (BSO) and Ba$_{1-x}$La$_x$SnO$_3$ (x = 7 %) (LBSO) thin films on different perovskite single crystal (SrTiO$_3$ (001) and SmScO$_3$ (110)) substrates has been achieved by Pulsed Laser Deposition (PLD) under optimized deposition conditions. X-ray diffraction measurements indicate that the films on either of these substrates are relaxed due to the large mismatch and present a high degree of crystallinity with narrow rocking curves and smooth surface morphology while analytical quantification by proton induced x-ray emission (PIXE) confirms the stoichiometric La transfer from a polyphasic target, producing films with La contents above the bulk solubility limit. The films show degenerate semiconducting behavior on both substrates, with the observed room temperature resistivities, Hall mobilities and carrier concentrations of 4.4 $m \Omega cm$, 10.11 $cm^2 V^{-1} s^{-1}$, and 1.38 $\cdot 10^{20} cm^{-3}$ on SmScO$_3$ and 7.8 $m \Omega cm$, 5.8 $cm^2 V^{-1} s^{-1}$, and 1.36 $\cdot 10^{20} cm^{-3}$ on SrTiO$_3$ ruling out any extrinsic contribution from the substrate. The superior electrical properties observed on the SmScO3 substrate are attributed to reduction in dislocation density from the lower lattice mismatch.
    05/2014;
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    ABSTRACT: Porous materials are attractive for separation and catalysis-these applications rely on selective interactions between host materials and guests. In metal-organic frameworks (MOFs), these interactions can be controlled through a flexible structural response to the presence of guests. Here we report a MOF that consists of glycyl-serine dipeptides coordinated to metal centres, and has a structure that evolves from a solvated porous state to a desolvated non-porous state as a result of ordered cooperative, displacive and conformational changes of the peptide. This behaviour is driven by hydrogen bonding that involves the side-chain hydroxyl groups of the serine. A similar cooperative closure (reminiscent of the folding of proteins) is also displayed with multipeptide solid solutions. For these, the combination of different sequences of amino acids controls the framework's response to the presence of guests in a nonlinear way. This functional control can be compared to the effect of single-point mutations in proteins, in which exchange of single amino acids can radically alter structure and function.
    Nature Chemistry 04/2014; 6(4):343-51. · 21.76 Impact Factor
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    ABSTRACT: A flexible metal-organic framework selectively sorbs para- (pX) over meta-xylene (mX) by synergic restructuring around pX coupled with generation of unused void space upon mX loading. The nature of the structural change suggests more generally that flexible structures which are initially mismatched in terms of fit and capacity to the preferred guest are strong candidates for effective molecular separations.
    Angewandte Chemie International Edition 03/2014; · 11.34 Impact Factor
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    ABSTRACT: The oxide heterostructure [(YFeO$_3$)$_5$(LaFeO$_3$)$_5$]$_{40}$, which is magnetically ordered and piezoelectric at room temperature, has been constructed from two weak ferromagnetic AFeO$_3$ perovskites with different A cations using RHEED-monitored pulsed laser deposition. The polarisation arises through the removal of inversion centres present within the individual AFeO$_3$ components. This symmetry reduction is a result of combining ordering on the A site, imposed by the periodicity of the grown structure, with appropriate orientations of the octahedral tilting characteristic of the perovskite units themselves, according to simple symmetry-controlled rules. The polarisation is robust against A site interdiffusion between the two layers which produces a sinusoidally modulated occupancy that retains the coupling of translational and point symmetries required to produce a polar structure. Magnetization and magneto-optical Kerr rotation measurements show that the heterostructure's magnetic structure is similar to that of the individual components. Evidence of the polarity was obtained from second harmonic generation and piezoelectric force microscopy measurements. Modeling of the piezoresponse allows extraction of $d_{33}$ (approximately 10 pC/N) of the heterostructure, which is in agreement with DFT calculations.
    Chemical Science 01/2014; 5:1599. · 8.31 Impact Factor
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    ABSTRACT: The functional properties of materials can arise from local structural features that are not well determined or described by crystallographic methods based on long-range average structural models. The room temperature (RT) structure of the Bi perovskite Bi2Mn4/3Ni2/3O6 has previously been modeled as a locally polar structure where polarization is suppressed by a long-range incommensurate antiferroelectric modulation. In this study we investigate the short-range local structure of Bi2Mn4/3Ni2/3O6, determined through reverse Monte Carlo (RMC) modeling of neutron total scattering data, and compare the results with the long-range incommensurate structure description. While the incommensurate structure has equivalent B site environments for Mn and Ni, the local structure displays a significantly Jahn?Teller distorted environment for Mn3+. The local structure displays the rock-salt-type Mn/Ni ordering of the related Bi2MnNiO6 high pressure phase, as opposed to Mn/Ni clustering observed in the long-range average incommensurate model. RMC modeling reveals short-range ferroelectric correlations between Bi3+ cations, giving rise to polar regions that are quantified for the first time as existing within a distance of approximately 12 Å. These local correlations persist in the commensurate high temperature (HT) phase, where the long-range average structure is nonpolar. The local structure thus provides information about cation ordering and B site structural flexibility that may stabilize Bi3+ on the A site of the perovskite structure and reveals the extent of the local polar regions created by this cation.
    Chem. Mater. 01/2014; 26(7):2218-2232.
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    ABSTRACT: Scandium perovskite (Sc0.94Mn0.06)Mn0.65Ni0.35O3, synthesized at high pressure and high temperature, has a triclinic structure (space group ) at room temperature and ambient pressure with a √2ap×√2ap×2ap structure with α≈90(°),β≈89(°),γ≈90(°). Magnetic measurements show that the material displays Curie-Weiss behaviour above 50 K with C=2.11 emu K mol(-1) (μeff=4.11 μB per formula unit) and θ=-95.27 K. Bond valence sum analysis of the crystal structure shows that manganese is present in three different oxidation states (+2, +3, +4), with the +2 oxidation state on the A site resulting in a highly tilted perovskite structure (average tilt 21.2(°) compared with 15.7(°) calculated for LaCaMnNbO6), giving the formula .
    Philosophical Transactions of The Royal Society A Mathematical Physical and Engineering Sciences 01/2014; 372(2013):20130012. · 2.89 Impact Factor
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    Journal of Physics and Chemistry of Solids 01/2014; · 1.53 Impact Factor
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    ABSTRACT: The alkali fullerides, A3C60 (A = alkali metal) are molecular superconductors that undergo a transition to a magnetic Mott-insulating state at large lattice parameters. However, although the size and the symmetry of the superconducting gap, Δ, are both crucial for the understanding of the pairing mechanism, they are currently unknown for superconducting fullerides close to the correlation-driven magnetic insulator. Here we report a comprehensive nuclear magnetic resonance (NMR) study of face-centred-cubic (f.c.c.) Cs3C60 polymorph, which can be tuned continuously through the bandwidth-controlled Mott insulator-metal/superconductor transition by pressure. When superconductivity emerges from the insulating state at large interfullerene separations upon compression, we observe an isotropic (s-wave) Δ with a large gap-to-superconducting transition temperature ratio, 2Δ0/kBTc = 5.3(2) [Δ0 = Δ(0 K)]. 2Δ0/kBTc decreases continuously upon pressurization until it approaches a value of ~3.5, characteristic of weak-coupling BCS theory of superconductivity despite the dome-shaped dependence of Tc on interfullerene separation. The results indicate the importance of the electronic correlations for the pairing interaction as the metal/superconductor-insulator boundary is approached.
    Scientific Reports 01/2014; 4:4265. · 5.08 Impact Factor
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    ABSTRACT: The peptide-based porous 3D framework, ZnCar, has been synthesized from Zn(2+) and the natural dipeptide carnosine (β-alanyl-L-histidine). Unlike previous extended peptide networks, the imidazole side chain of the histidine residue is deprotonated to afford Zn-imidazolate chains, with bonding similar to the zeolitic imidazolate framework (ZIF) family of porous materials. ZnCar exhibits permanent microporosity with a surface area of 448 m(2) g(-1) , and its pores are 1D channels with 5 Å openings and a characteristic chiral shape. This compound is chemically stable in organic solvents and water. Single-crystal X-ray diffraction (XRD) showed that the ZnCar framework adapts to MeOH and H2 O guests because of the torsional flexibility of the main His-β-Ala chain, while retaining the rigidity conferred by the Zn-imidazolate chains. The conformation adopted by carnosine is driven by the H bonds formed both to other dipeptides and to the guests, permitting the observed structural transformations.
    Angewandte Chemie International Edition 12/2013; · 11.34 Impact Factor
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    ABSTRACT: NiO:Li is an early exemplar for which hole-doping of a correlated insulator gives rise to rich and varied magnetic behavior. It is also an important system from the viewpoint of p-type transparent conducting oxides, and is representative of a large class of materials that have been used in lithium ion batteries, since the end-member compound, LiNiO2 , belongs to the class of layered cathode materials. Despite the deceptive structural and compositional simplicity of this system, a complete understanding of its complex magnetic properties has remained elusive. Here a comprehensive investigation of the solid solution Lix Ni2-x O2 , examining samples of precise stoichiometry using a combination of high-resolution synchrotron X-ray powder diffraction and SQUID magnetometry, is provided. The focus is on the interesting region between 0.40<x<1.00 in which the magnetic ordering temperature changes drastically with composition. The magnetism evolves from strong G-type antiferromagnetism of x=0.40 with TN =327 K to robust uncompensated magnetic order at TN =240 K when x is close to 0.7, and to glassy A-type antiferromagnetism of x=1.00 at TN =9 K. This study demonstrates this magnetic behavior is linked to the Li-Ni chemical order that develops from short- to long-range. The interfaces between ordered domains give rise to magnetic exchange bias, which manifests as a shift in the magnetization-field loop for samples with nanoscale coherence lengths (0.54<x<0.66).
    Chemistry 09/2013; · 5.93 Impact Factor

Publication Stats

6k Citations
2,123.05 Total Impact Points

Institutions

  • 2003–2014
    • University of Liverpool
      • Department of Chemistry
      Liverpool, England, United Kingdom
  • 2011–2013
    • University of California, Santa Barbara
      • Materials Research Laboratory
      Santa Barbara, CA, United States
    • Heriot-Watt University
      • Department of Chemical Engineering
      Edinburgh, SCT, United Kingdom
    • Sun Yat-Sen University
      • Department of Chemical Engineering
      Shengcheng, Guangdong, China
  • 2012
    • Hungarian Academy of Sciences
      • Institute for Solid State Physics and Optics
      Budapest, Budapest fovaros, Hungary
  • 1999–2010
    • University of Exeter
      Exeter, England, United Kingdom
  • 1988–2010
    • University of Oxford
      • • Inorganic Chemistry Laboratory
      • • Department of Physics
      • • Department of Chemistry
      Oxford, England, United Kingdom
  • 2007–2009
    • Durham University
      • Department of Chemistry
      Durham, ENG, United Kingdom
    • Beverly Hospital, Boston MA
      Beverly, Massachusetts, United States
  • 2006
    • Boston College, USA
      Boston, Massachusetts, United States
  • 2004
    • Newcastle University
      • School of Chemistry
      Newcastle-on-Tyne, England, United Kingdom
  • 2003–2004
    • The University of Sheffield
      • Department of Materials Science and Engineering
      Sheffield, England, United Kingdom
  • 1989
    • Institut Laue-Langevin
      Grenoble, Rhône-Alpes, France