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Instruments / Technical Area	Publication Details	Published
I15-Extreme Conditions	Exfoliation of layered Na-ion anode material Na 2 Ti 3 O 7 for enhanced capacity and cyclability Maria A. Tsiamtsouri , Phoebe K. Allan , Andrew J. Pell , Joshua M. Stratford , Gunwoo Kim , Rachel N. Kerber , Pieter M. Magusin , David A. Jefferson , Clare P. Grey Chemistry Of Materials DOI: 10.1021/acs.chemmater.7b03753 Diamond Proposal Number(s): [14177] Show Abstract ▼ Abstract: We report the exfoliation of layered Na2Ti3O7, a promising anode material for Na-ion batteries, and restacking using HNO3 and NaOH to form H-[Ti3O7] and Na(x)-[Ti3O7] compositions, respectively. The materials were characterised by a range of techniques (SEM, TEM, solid state NMR, XRD, PDF). Although the formation of aggregated nanoparticles is favoured under acidic restacking conditions, control over the adherence between the exfoliated layers can be achieved in basic conditions. Pair distribution function (PDF) analysis confirms that the local TiO6 connectivity of the pristine material is maintained. The lowest sodium-containing Na(1)-[Ti3O7] phase, which is the stable product upon Na+ leaching after consecutive washing steps, displays the best performance among the compositions studied, affording a stable reversible capacity of about 200 mAh.g-1 for 20 cycles at a C/20 rate. Washing removes the excess of ‘free/reactive’ Na+, which otherwise forms inactive Na2CO3 in the insufficiently-washed compositions.	Feb 2018
I11-High Resolution Powder Diffraction	Single Sublattice Endotaxial Phase Separation Driven by Charge Frustration in a Complex Oxide Antoine Demont , Ruth Sayers , Maria Tsiamtsouri , Simon Romani , Philip Chater , Hongjun Niu , Carlos Martí-gastaldo , Zhongling Xu , Zengqiang Deng , Yohann Bréard , Michael F. Thomas , John Claridge , Matthew Rosseinsky Journal Of The American Chemical Society 135 (27), 10114 - 10123 DOI: 10.1021/ja403611s Open Access Show Abstract ▼ Abstract: Complex transition-metal oxides are important functional materials in areas such as energy and information storage. The cubic ABO3 perovskite is an archetypal example of this class, formed by the occupation of small octahedral B-sites within an AO3 network defined by larger A cations. We show that introduction of chemically mismatched octahedral cations into a cubic perovskite oxide parent phase modifies structure and composition beyond the unit cell length scale on the B sublattice alone. This affords an endotaxial nanocomposite of two cubic perovskite phases with distinct properties. These locally B-site cation-ordered and -disordered phases share a single AO3 network and have enhanced stability against the formation of a competing hexagonal structure over the single-phase parent. Synergic integration of the distinct properties of these phases by the coherent interfaces of the composite produces solid oxide fuel cell cathode performance superior to that expected from the component phases in isolation.	Jul 2013
I11-High Resolution Powder Diffraction	Stabilization of a Complex Perovskite Superstructure under Ambient Conditions: Influence of Cation Composition and Ordering, and Evaluation as an SOFC Cathode A. Demont , M. S. Dyer , R. Sayers , M. F. Thomas , M. Tsiamtsouri , H. N. Niu , G. R. Darling , A. Daoud-aladine , J. B. Claridge , M. J. Rosseinsky Chemistry Of Materials 22 (24), 65986615 DOI: 10.1021/cm102475n Open Access Show Abstract ▼ Abstract: Ba1.6Ca2.3Y1.1Fe5O13 is an Fe3+ oxide adopting a complex perovskite superstructure, which is an ordered intergrowth between the Ca2Fe2O5 and YBa2Fe3O8 structures featuring octahedral, square pyramidal, and tetrahedral B sites and three distinct A site environments. The distribution of A site cations was evaluated by combined neutron and X-ray powder diffraction. Consistent with the Fe3+ charge state, the material is an antiferromagnetic insulator with a Nel temperature of 480−485 °C and has a relatively low d.c. conductivity of 2.06 S cm−1 at 700 °C. The observed area specific resistance in symmetrical cell cathodes with the samarium-doped ceria electrolyte is 0.87 Ω cm2 at 700 °C, consistent with the square pyramidal Fe3+ layer favoring oxide ion formation and mobility in the oxygen reduction reaction. Density functional theory calculations reveal factors favoring the observed cation ordering and its influence on the electronic structure, in particular the frontier occupied and unoccupied electronic states.	Dec 2010

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