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89 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5, 6, 7, 8 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	Gold(i) bridged dimeric and trimeric heterometallic {Cr7Ni}-based qubit systems and their characterization Deepak Asthana , Selena J. Lockyer , Selina Nawaz , Robert J. Woolfson , Grigore A. Timco , Christopher A. Muryn , Iñigo J. Vitorica-Yrezabal , David Collison , Neil A. Burton , Richard E. P. Winpenny Dalton Transactions 42 DOI: 10.1039/D1DT00150G Diamond Proposal Number(s): [23480] Open Access Show Abstract ▼ Abstract: Gold(I) bridged dimeric and trimeric structures of a ground state spin S = 1/2 heterometallic {Cr7Ni} wheel have been prepared and studied by continuous wave (CW) and pulsed wave EPR spectrometry. The {Cr7Ni} relaxation time constants (T1 and Tm) show rates matching well with previous observations. Four pulse Double Electron Resonance (DEER) studies suggest presence of more than one conformations. Small Angle X-ray Scattering (SAXS) in conjunction with Molecular Dynamic (MD) Simulations were performed to look at the possible conformations in solution. In line with DEER results, simulation data further indicated more flexible molecular geometry in solution than the one in solid state.	Mar 2021
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF)	Stepwise collapse of a giant pore metal–organic framework Adam F. Sapnik , Duncan N. Johnstone , Sean M. Collins , Giorgio Divitini , Alice M. Bumstead , Christopher W. Ashling , Philip A. Chater , Dean S. Keeble , Timothy Johnson , David A. Keen , Thomas D. Bennett Dalton Transactions 38 DOI: 10.1039/D1DT00881A Diamond Proposal Number(s): [20038, 20198] Open Access Show Abstract ▼ Abstract: Defect engineering is a powerful tool that can be used to tailor the properties of metal–organic frameworks (MOFs). Here, we incorporate defects through ball milling to systematically vary the porosity of the giant pore MOF, MIL-100 (Fe). We show that milling leads to the breaking of metal–linker bonds, generating additional coordinatively unsaturated metal sites, and ultimately causes amorphisation. Pair distribution function analysis shows the hierarchical local structure is partially retained, even in the amorphised material. We find that solvents can be used to stabilise the MIL-100 (Fe) framework against collapse, which leads to a substantial retention of porosity over the non-stabilised material.	Mar 2021
I19-Small Molecule Single Crystal Diffraction	Unveiling the role of the lone electron pair in sesquioxides at high pressure: compressibility of β-Sb2O3 Juan Angel Sans , Francisco Javier Manjon , André Luis De Jesus Pereira , Javier Ruiz-Fuertes , Catalin Popescu , Alfonso Muñoz , Plácida Rodríguez-Hernández , Julio Pellicer-Porres , Vanesa Paula Cuenca-Gotor , Julia Contreras-Garcia , Jordi Ibañez , Virginia Monteseguro Dalton Transactions 854 DOI: 10.1039/D1DT00268F Diamond Proposal Number(s): [22223] Show Abstract ▼ Abstract: The structural, vibrational and electronic properties of the compressed β-Sb2O3 polymorph, a.k.a. mineral valentinite, have been investigated in a joint experimental and theoretical study up to 23 GPa. The compressibility of the lattice parameters, unit-cell volume and polyhedral unit volume as well as the behaviour of its Raman- and IR-active modes under compression have been interpreted on the basis of ab initio theoretical simulations. Valentinite shows an unusual compressibility up to 15 GPa with four different pressure ranges, whose critical pressures are 2, 4, and 10 GPa. The pressure dependence of the main structural units, the lack of soft phonons, and the electronic density charge topology address the changes at those critical pressures to isostructural phase transitions of degree higher than 2. In particular, the transitions at 2 and 4 GPa can be ascribed to the changes in the interaction between the stereochemically-active lone electron pairs of Sb atoms under compression. The changes observed above 10 GPa, characterized by a general softening of several Raman- and IR-active modes, point to a structural instability prior to the 1st-order transition occurring above 15 GPa. Above this pressure, a tentative new high-pressure phase (s.g. Pcc2) has been assigned by single-crystal and powder X-ray diffraction measurements.	Mar 2021
I19-Small Molecule Single Crystal Diffraction	Phosphido-bis(borane) complexes of the alkaline earth metals Keith Izod , James M. Watson , Ross W. Harrington , William Clegg Dalton Transactions 50, 1019-1024 DOI: 10.1039/D0DT03895D Diamond Proposal Number(s): [6302] Show Abstract ▼ Abstract: The reaction between two equivalents of {(Me3Si)2CH}(Ph)PH(BH3) (1) and Bu2Mg, followed by two equivalents of BH3·SMe2, gives the corresponding phosphido-bis(borane) complex, which may be crystallised as two distinct chemical species: the complex [{(Me3Si)2CH}(Ph)P(BH3)2]2Mg(THF)4·THF (2a), and two different THF solvates (1 : 1 and 1 : 2) of the solvent-separated ion triples [{(Me3Si)2CH}(Ph)P(BH3)2]2[Mg (THF)6]·THF (2b) and [{(Me3Si)2CH}(Ph)P(BH3)2]2[Mg(THF)6]·2THF (2c). Similar reactions between two equivalents of 1 and either (4-tBuC6H4CH2)2Ca(THF)4 or [(Me3Si)2CH]2Sr(THF)2, followed by two equivalents of BH3·SMe2, give the heavier alkali metal complexes [{(Me3Si)2CH}(Ph)P(BH3)2]2M(THF)4 [M = Ca (3), Sr (4)]. Surprisingly, compounds 2a, 3 and 4 adopt almost identical structures in the solid state, which differ only in the geometrical arrangement of the phosphido-bis(borane) ligands and the hapticity of the borane groups.	Dec 2020
I19-Small Molecule Single Crystal Diffraction	Phthalocyanine-polyoxotungstate lanthanide double deckers Sidra Sarwar , Sergio Sanz , Jan Van Leusen , Gary S. Nichol , Euan K. Brechin , Paul Kögerler Dalton Transactions 25, 16638-16642 DOI: 10.1039/D0DT03716H Diamond Proposal Number(s): [22240] Show Abstract ▼ Abstract: Acetate ligand metathesis results in the first hybrid [MIII(Pc)(PW11O39)]6− (M = Y, Dy, Tb) double-decker scaffolds, where a phthalocyanate (Pc2−) and one of the conceptually most simple polyoxotungstates, a monolacunary Keggin cluster, are interlinked via a single rare earth ion. Characterisation includes high-resolution mass spectrometry, synchrotron-based single-crystal X-ray diffraction, various spectroscopic and electrochemical methods, and magnetic studies revealing slow relaxation of the magnetisation for the Dy derivate.	Nov 2020
I11-High Resolution Powder Diffraction	Structural variations in (001)-oriented layered lead halide perovskites, templated by 1,2,4-triazolium Yuan-yuan Guo , Lin-jie Yang , Jason A. Mcnulty , Alexandra M. Z. Slawin , Philip Lightfoot Dalton Transactions 119 DOI: 10.1039/D0DT02936J Diamond Proposal Number(s): [23579] Show Abstract ▼ Abstract: A new hybrid lead(II) halide perovskite, (TzH)2PbCl4, ([TzH+] = 1,2,4-triazolium), adopts a (001)-oriented layered perovskite structure, which can be considered as derived from the n = 1 Ruddlesden–Popper (RP) type. Variable temperature single crystal X-ray diffraction reveals a structural phase transition in the region 125 K < T < 173 K between a high temperature, high symmetry polymorph, space group Cmcm, and a low temperature, low symmetry chiral polymorph, space group P212121, which has a tripled unit cell volume. UV-Vis spectra suggest a band gap of 3.30 eV for (TzH)2PbCl4. A second polymorph of the bromide analogue, (TzH)2PbBr4-II, is also reported, and structural relationships between all three variants are discussed.	Nov 2020
B18-Core EXAFS I11-High Resolution Powder Diffraction	Ce(OH)2Cl and lanthanide-substituted variants as precursors to redox-active CeO2 materials Alexander J. A. Dunn , James W. Annis , Janet M. Fisher , David Thompsett , Richard Walton Dalton Transactions 38 DOI: 10.1039/D0DT03435E Diamond Proposal Number(s): [14239, 18786] Open Access Show Abstract ▼ Abstract: The cerium(III) hydroxide chloride Ce(OH)2Cl crystallises directly as a polycrystalline powder from a solution of CeCl3·7H2O in poly(ethylene) glycol (Mn = 400) heated at 240 °C and is found to be isostructural with La(OH)2Cl, as determined from high-resolution synchrotron powder X-ray diffraction (P21/m, a = 6.2868(2) Å, b = 3.94950(3) Å, c = 6.8740(3) Å, β = 113.5120(5)°). Replacement of a proportion of the cerium chloride in synthesis by a second lanthanide chloride yields a set of materials Ce1−xLnx(OH)2Cl for Ln = La, Pr, Gd, Tb. For La the maximum value of x is 0.2, with an isotropic expansion of the unit cell, but for the other lanthanides a wider composition range is possible, and the lattice parameters show an isotropic contraction with increasing x. Thermal decomposition of the hydroxide chlorides at 700 °C yields mixed-oxides Ce1−xLnxO2−δ that all have cubic fluorite structures with either expanded (Ln = La, Gd) or contracted (Ln = Pr, Tb) unit cells compared to CeO2. Scanning electron microscopy shows a shape memory effect in crystal morphology upon decomposition, with clusters of anisotropic sub-micron crystallites being seen in the precursor and oxide products. The Pr- and Tb-substituted oxides contain the substituent in a mixture of +3 and +4 oxidation states, as seen by X-ray absorption near edge structure spectroscopy at the lanthanide LIII edges. The mixed oxide materials are examined using temperature programmed reduction in 10%H2 in N2, which reveals redox properties suitable for heterogeneous catalysis, with the Pr-substituted materials showing the greatest reducibility at lower temperature.	Oct 2020
I15-Extreme Conditions	Spin crossover in the Prussian blue analogue FePt(CN) 6 induced by pressure or X-ray irradiation Hanna L. B. Bostroem , Andrew B. Cairns , Lei Liu , Peter Lazor , Ines E. Collings Dalton Transactions 49, 12940 - 12944 DOI: 10.1039/D0DT02036B Diamond Proposal Number(s): [19776] Open Access Show Abstract ▼ Abstract: The spin state of the Prussian blue analogue FeIIPtIV(CN)6 is investigated in response to temperature, pressure, and X-ray irradiation. While cooling to 10 K maintains the high-spin state of FeII, compression at ambient temperature induces a first-order spin-crossover (SCO) transition with a small hysteresis loop (p↑ = 0.8 GPa, p↓ = 0.6 GPa). In addition, the high-spin to low-spin transition can be initiated at lower pressure through increased X-ray irradiation. Our study highlights a cooperative SCO with moderate pressure in a porous Prussian blue analogue.	Sep 2020
I11-High Resolution Powder Diffraction	Mn2+ luminescence of Gd(Zn,Mg)B5O10 pentaborate under high pressure Lev-ivan Bulyk , Leonid Vasylechko , Vitaliy Mykhaylyk , Chiu C. Tang , Yaroslav Zhydachevskii , Yuriy Hizhnyi , Sergiy G. Nedilko , Nickolai Klyui , Andrzej Suchocki Dalton Transactions DOI: 10.1039/D0DT01851A Show Abstract ▼ Abstract: Results of X-ray diffraction studies of Gd(Mg0.95 x,ZnxMn 0.05)B5O10 down-converting phosphor as a function of Mg-Zn composition are presented. Lattice parameters and unit cell volumes of GdMg0.95-xZnxMn0.05B5O10 pentaborates are examined. The relationships between the structure and optical properties of these materials are explicated based on the results of theoretical calculations of the energy structure. The effect of pressure on the luminescence of Mn2+ in this system was studied up to ca. 32 GPa. The observed quenching of Mn2+ luminescence is due to crossing of the emitting 4T1g level with the non-emitting 2T2g state. This crossing sets the long-wavelength limit on the possibility of observation the emission of Mn2+ ion, which is around 850 nm.	Sep 2020
I19-Small Molecule Single Crystal Diffraction	Hydrogen peroxide assisted photorelease of an anthraquinone-based ligand from [Ru(2,2′-bipyridine) 2 (9,10-dioxo-9,10-dihydroanthracen-1-olate)]Cl in aqueous solution L. Zeng , D. Sirbu , P. G. Waddell , N. V. Tkachenko , M. R. Probert , A. C. Benniston Dalton Transactions 129 DOI: 10.1039/D0DT02339F Diamond Proposal Number(s): [22240] Open Access Show Abstract ▼ Abstract: A new class of light-activated ruthenium(II) complex was designed as a potential blocker of biological functioning, especially for targeting redox reactions within mitochondria under light activation. Based on our concepts the complex [Ru(bipy)2(1-hydroxyanthra-9,10 quinone)]Cl (RU1) was prepared and studied to understand the preliminary reaction mechanisms and its excited state behaviour through a series of stability tests, electrochemistry, UV–Visible kinetics and femtosecond transient absorption spectroscopy experiments. Under white light in the presence of H2O2 two different reactions (fast and slow) appear to take place. The complex loses the quinone-based ligand and a resulting Ru(III) or Ru(V) species is produced. The complex RU1 shows potential to consume H2O2 from the one carbon metabolism in mitochondria, and hence may cut the energy cycle pathway of tumor cells.	Aug 2020

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