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11 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	Multivariate metal−organic frameworks for the simultaneous capture of organic and inorganic contaminants from water Marta Mon , Rosaria Bruno , Estefanía Tiburcio , Marta Viciano-chumillas , Lucas H. G. Kalinke , Jesus Ferrando-soria , Donatella Armentano , Emilio Pardo Journal Of The American Chemical Society DOI: 10.1021/jacs.9b06250 Diamond Proposal Number(s): [22411] Show Abstract ▼ Abstract: We report a new water-stable multivariate (MTV) Metal-Organic Framework (MOF) prepared by combining two different oxamide-based metalloligands derived from the natural amino acids L-serine and L-methionine. This unique material features hexagonal channels decorated with two types of flexible and functional “arms” (–CH2OH and –CH2CH2SCH3) capa-ble to act, synergistically, for the simultaneous and efficient removal of both inorganic (heavy metals like Hg2+, Pb2+ and Tl+) and organic (dyes such as Pyronin Y, Auramine O, Brilliant Green and Methylene Blue) contaminants and, in addi-tion, this MTV-MOF is completely reusable. Single-crystal X-ray diffraction (SCXRD) measurements allowed to solve the crystal structure of a host-guest adsorbate, containing both HgCl2 and Methylene Blue, and offered unprecedented snap-shots about this unique dual capture process. This is the very first time that a MOF can be used for the removal of all sorts of pollutants from water resources, thus opening new perspectives for this emerging type of MTV-MOFs.	Aug 2019
I19-Small Molecule Single Crystal Diffraction	A [13]rotaxane assembled via a palladium molecular capsule Jesus Ferrando-soria , Antonio Fernandez , Deepak Asthana , Selina Nawaz , Iñigo J. Vitorica-yrezabal , George F. S. Whitehead , Christopher A. Muryn , Floriana Tuna , Grigore A. Timco , Neil D. Burton , Richard E. P. Winpenny Nature Communications 10 DOI: 10.1038/s41467-019-11635-6 Open Access Show Abstract ▼ Abstract: Molecules that are the size of small proteins are difficult to make. The most frequently examined route is via self-assembly, and one particular approach involves molecular nanocapsules, where ligands are designed that will enforce the formation of specific polyhedra of metals within the core of the structure. Here we show that this approach can be combined with mechanically interlocking molecules to produce nanocapsules that are decorated on their exterior. This could be a general route to very large molecules, and is exemplified here by the synthesis and structural characterization of a [13]rotaxane, containing 150 metal centres. Small angle X-ray scattering combined with atomistic molecular dynamics simulations demonstrate the compound is intact in solution.	Aug 2019
I19-Small Molecule Single Crystal Diffraction	Efficient gas separation and transport mechanism in rare hemilabile metal-organic framework Marta Mon , Rosaria Bruno , Estefanía Tiburcio , Aida Grau-atienza , Antonio Sepulveda-escribano , Enrique V Ramos-fernandez , Alessio Fuoco , Elisa Esposito , Marcello Monteleone , Johannes Carolus Jansen , Joan Cano , Jesus Ferrando-soria , Donatella Armentano , Emilio Pardo Chemistry Of Materials DOI: 10.1021/acs.chemmater.9b01995 Diamond Proposal Number(s): [18768] Show Abstract ▼ Abstract: Understand/visualize the established interactions between gases and adsorbents is mandatory to implement better per-formant materials in adsorption/separation processes. Here we report the unique behavior of a rare example of a hemila-bile chiral three-dimensional metal-organic framework (MOF) with an unprecedented qtz-e-type topology, with formula CuII2(S,S)-hismox . 5H2O (1) (hismox = bis[(S)-histidine]oxalyl diamide). 1 exhibits a continuous and reversible breath-ing behavior, based on the hemilability of carboxylate groups from L-histidine. In-situ powder (PXRD) and single crystal X-ray diffraction (SCXRD) using synchrotron radiation allowed to unveil the crystal structures of 4 different host-guest adsorbates (Ar, N2, CO2 and C3H6@1), the rationalization of the breathing motion and unravel the mechanisms govern-ing the adsorption of these gases. Then, this information has been transferred to implement efficient separations of mix-tures of industrial and environmental relevance –CO2/N2, CO2/CH4 and C3H8/C3H6 using 1 in packed columns as the sta-tionary phase and dispersed in a mixed matrix membrane.	Jul 2019
I19-Small Molecule Single Crystal Diffraction	Self-assembly of catalytically-active supramolecular coordination compounds within metal-organic frameworks Rosa Adam , Marta Mon , Lucas H. G. Kalinke , Alejandro Vidal-moya , Antonio Fernandez , Richard E. P. Winpenny , Antonio Domenech-carbo , Antonio Leyva-perez , Donatella Armentano , Emilio Pardo , Jesus Ferrando-soria Journal Of The American Chemical Society DOI: 10.1021/jacs.9b03914 Diamond Proposal Number(s): [18768] Show Abstract ▼ Abstract: Supramolecular Coordination Compounds (SCCs) represent the power of Coordination Chemistry methodologies to self-assemble discrete architectures with targeted properties. SCCs are generally synthesised in solution, with isolat-ed fully-coordinated metal atoms as structural nodes, thus severely limited as metal-based catalysts. Metal-Organic Frameworks (MOFs) show unique features to act as chemical nanoreactors for the in-situ synthesis and stabilization of otherwise not accessible functional species. Here, we present the self-assembly of PdII SCCs within the confined space of a preformed MOF (SCCs@MOF) and its post-assembly metalation to give a PdII-AuIII supramolecular assembly, crys-tallography underpinned. These SCCs@MOF catalyse the coupling of boronic acids and/or alkynes, representative multisite metallic-catalysed reactions in which traditional SCCs tend to decompose, and retain its structural integrity as consequence of the synergetic hybridization between SCCs and MOF. These results open new avenues in both the synthesis of novel SCCs and their use on heterogeneous metal-based Supramolecular Catalysis.	Jun 2019
I19-Small Molecule Single Crystal Diffraction	Formation of an interlocked double-chain from an organic–inorganic [2]rotaxane Jesus Ferrando Soria , Antonio Fernandez , Iñigo J. Vitorica-yrezabal , Deepak Asthana , Christopher A. Muryn , Floriana Tuna , Grigore A. Timco , Richard E. P. Winpenny Chemical Communications 111 DOI: 10.1039/C8CC09339C Show Abstract ▼ Abstract: Here we show that a structure containing a polymeric interlocking daisy chain is obtained from the reaction of an inorganic–organic [2]rotaxane [HB{CrIII7NiII(μ-F)8(O2CtBu)16}], where B is an organic thread terminated with a bi-pyridyl unit, with an oxo-centered metal carboxylate triangle [FeIII2CoII(μ3-O)(O2CtBu)6(HO2CtBu)3].	Feb 2019
I19-Small Molecule Single Crystal Diffraction	Confined Pt11+–water clusters in a MOF catalyze the low–temperature water–gas shift reaction with waterborne co2 oxygen atoms Emilio Pardo , Donatella Armentano , Miguel A. Rivero–crespo , Marta Mon Conejero , Jesus Ferrando-soria , Christian W. Lopes , Mercedes Boronat , Antonio Leyva–pérez , Avelino Corma , Juan C. Hernández–garrido , Miguel López–haro , Jose J. Calvino , Enrique V. Ramos–fernandez Angewandte Chemie International Edition DOI: 10.1002/anie.201810251 Diamond Proposal Number(s): [16033, 18768] Show Abstract ▼ Abstract: The synthesis and reactivity of single metal atoms in low–valence state bound to just water, rather than to organic ligands or surfaces, is conceptually relevant and a major experimental challenge. Here, we show a gram–scale wet synthesis of a Pt11+ complex stabilized in a confined space by a water cluster, formed by a well–defined crystallographic first water sphere and a second coordination sphere linked to a Metal–Organic Framework (MOF) through electrostatic and H–bonding interactions. The role of the water cluster is not only isolating and stabilizing the Pt atoms, but also regulating the charge of the metal and the adsorption of reactants. This is shown for the low–temperature water–gas shift reaction (WGSR: CO + H2O → CO2 + H2), where both metal coordinated and H–bonded water molecules trigger a double water attack mechanism to CO and give CO2 with both oxygen atoms coming from water. The stabilized Pt1+ single sites in confined water clusters allow performing the WGSR at temperatures as low as 50 ºC.	Nov 2018
I19-Small Molecule Single Crystal Diffraction	Fine-tuning of the confined space in microporous metal–organic frameworks for efficient mercury removal Marta Mon , Xiaoni Qu , Jesus Ferrando-soria , Isaac Pellicer-carreño , Antonio Sepulveda-escribano , Enrique V. Ramos-fernandez , Johannes C. Jansen , Donatella Armentano , Emilio Pardo J. Mater. Chem. A 251 DOI: 10.1039/C7TA06199D Diamond Proposal Number(s): [15244] Show Abstract ▼ Abstract: Offsetting the impact of human activities on the biogeochemical cycle of mercury has become necessary for a sustainable planet. Herein, we report the development of a water-stable and eco-friendly metal–organic framework, which has the formula {Cu4 II[(S,S)-methox]2}. 5H2O (1), where methox is bis[(S)-methionine]oxalyl diamide. Its features include narrow functional channels decorated with thioalkyl chains, which are able to capture HgCl2 from aqueous media in an efficient, selective, and rapid manner. The conscious design effort in terms of size, shape, and reactivity of the channels results in extremely efficient immobilization of HgCl2 guest species in a very stable conformation, similar to that of the enzyme mercury reductase. Thus, 1 enables the highly efficient removal of toxic HgCl2 from aqueous media and reduces the [Hg2+] concentration from the dangerous level of 10 ppm to acceptable limits of below 2 ppb in drinking water. The unusual combination of a low-cost straightforward synthetic procedure and high stability under environmental conditions, together with its ability to efficiently and rapidly remove poisonous mercury ions, places 1 among themost attractive adsorbents reported to date for the purification of contaminated water.	Aug 2017
I19-Small Molecule Single Crystal Diffraction	Switchable Interaction in Molecular Double Qubits Jesus Ferrando Soria , Samantha a. Magee , Alessandro Chiesa , Stefano Carretta , Paolo Santini , Inigo Vitorica-yrezabal1 , Floriana Tuna , George F. S. Whitehead , Stephen Sproules , Kyle m. Lancaster , Anne-laure Barra , Grigore a. Timco , Eric J. L. Mcinnes , Richard e. P. Winpenny Chem 1, 727 - 752 DOI: 10.1016/j.chempr.2016.10.001 Open Access Show Abstract ▼ Abstract: Quantum information processing (QIP) could revolutionize how we simulate and understand quantum systems. Any QIP scheme requires both individual units (qubits) that have long phase memories and switchable units that can be placed between the qubits. Here, we describe supramolecular systems where {Cr7Ni} rings are used as qubits, linked by redox-switchable {Ru2M} oxo-centered triangles (M = Zn, Ni, or Co). The supramolecular assemblies have been structurally characterized and involve two {Cr7Ni} rings bound to {Ru2M} triangles through iso-nicotinate ligands. Detailed physical studies, including electrochemistry and electron paramagnetic resonance spectroscopy, show that when M = Co, the supramolecular assembly has the physical characteristics needed to implement the √iSWAP gate, which is an important entangling two-qubit gate. Detailed simulations show that the fidelity of this gate is potentially very high and depends on the phase memory time of the {Cr7Ni} qubits but not the {Ru2Co} switch.	Nov 2016
I19-Small Molecule Single Crystal Diffraction	Making hybrid [n]-rotaxanes as supramolecular arrays of molecular electron spin qubits Antonio Fernandez , Jesus Ferrando Soria , Eufemio Moreno Pineda , Floriana Tuna , Iñigo J. Vitorica-yrezabal , Christiane Knappke , Jakub Ujma , Chris Muryn , Grigore A. Timco , Perdita E. Barran , Arzhang Ardavan , Richard E P Winpenny Nature Communications 7 DOI: 10.1038/ncomms10240 Open Access Show Abstract ▼ Abstract: Quantum information processing (QIP) would require that the individual units involved—qubits—communicate to other qubits while retaining their identity. In many ways this resembles the way supramolecular chemistry brings together individual molecules into interlocked structures, where the assembly has one identity but where the individual components are still recognizable. Here a fully modular supramolecular strategy has been to link hybrid organic–inorganic [2]- and [3]-rotaxanes into still larger [4]-, [5]- and [7]-rotaxanes. The ring components are heterometallic octanuclear [Cr7NiF8(O2CtBu)16]– coordination cages and the thread components template the formation of the ring about the organic axle, and are further functionalized to act as a ligand, which leads to large supramolecular arrays of these heterometallic rings. As the rings have been proposed as qubits for QIP, the strategy provides a possible route towards scalable molecular electron spin devices for QIP. Double electron–electron resonance experiments demonstrate inter-qubit interactions suitable for mediating two-qubit quantum logic gates.	Jan 2016
I19-Small Molecule Single Crystal Diffraction	Controlled Synthesis of Nanoscopic Metal Cages Jesus Ferrando Soria , Antonio Fernandez , Eufemio Moreno , Sarah A. Varey , Ralph W. Adams , Iñigo J. Vitorica-yrezabal , Floriana Tuna , Grigore A. Timco , Chris Muryn , Richard E. P. Winpenny Journal Of The American Chemical Society 137 (24), 7644 - 7647 DOI: 10.1021/jacs.5b04664 Diamond Proposal Number(s): [8977] Open Access Show Abstract ▼ Abstract: Here we show an elegant and general route to the assembly of a giant {M12C24} cage from 12 palladium ions (M) and 24 heterometallic octanuclear coordination cages (C = {Cr7Ni-Py2}). The molecule is 8 nm in size, and the methods for its synthesis and characterization provide a basis for future developments at this scale.	Jun 2015

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