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82 items found (0 items not approved), displaying 71 to 80.[First/Prev] 2, 3, 4, 5, 6, 7, 8, 9 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	Cation- and anion-exchanges induce multiple distinct rearrangements within metallosupramolecular architectures Imogen A. Riddell , Tanya Ronson , Jack K. Clegg , Christopher Wood , Rana A. Bilbeisi , Jonathan R. Nitschke Journal Of The American Chemical Society 136 (26) DOI: 10.1021/ja504748g Diamond Proposal Number(s): [7984, 8464] Show Abstract ▼ Abstract: Different anionic templates act to give rise to four distinct CdII-based architectures: a Cd2L3 helicate, a Cd8L12 distorted cuboid, a Cd10L15 pentagonal prism, and a Cd12L18 hexagonal prism, which respond to both anionic and cationic components. Interconversions between architectures are driven by the addition of anions that bind more strongly within a given product framework. The addition of FeII prompted metal exchange and transformation to a Fe4L6 tetrahedron or a Fe10L15 pentagonal prism, depending on the anionic templates present. The equilibrium between the Cd12L18 prism and the Cd2L3 triple helicate displayed concentration dependence, with higher concentrations favoring the prism. The Cd12L18 structure serves as an intermediate en route to a hexafluoroarsenate-templated Cd10L15 complex, whereby the structural features of the hexagonal prism preorganize the system to form the structurally related pentagonal prism. In addition to the interconversion pathways investigated, we also report the single-crystal X-ray structure of bifluoride encapsulated within a Cd10L15 complex and report solution state data for J-coupling through a CH···F– hydrogen bond indicating the strength of these interactions in solution.	Jun 2014
I19-Small Molecule Single Crystal Diffraction	Post-assembly modification of kinetically metastable FeII2L3 triple helicates Derrick A. Roberts , Ana M Castilla , Tanya Ronson , Jonathan R. Nitschke Journal Of The American Chemical Society 136 (23) DOI: 10.1021/ja5042397 Diamond Proposal Number(s): [8464] Open Access Show Abstract ▼ Abstract: We report the covalent post-assembly modification of kinetically metastable amine-bearing FeII2L3 triple helicates via acylation and azidation. Covalent modification of the metastable helicates prevented their reorganization to the thermodynamically favored FeII4L4 tetrahedral cages, thus trapping the system at the non-equilibrium helicate structure. This functionalization strategy also conveniently provides access to a higher-order tris(porphyrinatoruthenium)–helicate complex that would be difficult to prepare by de novo ligand synthesis.	May 2014
I19-Small Molecule Single Crystal Diffraction	Selective encapsulation and sequential release of guests within a self-sorting mixture of three tetrahedral cages Azucena Jiménez , Rana A. Bilbeisi , Tanya Ronson , Salvatore Zarra , Craig Woodhead , Jonathan R. Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.201400541 PMID: 24692286 Diamond Proposal Number(s): [7569] Show Abstract ▼ Abstract: A mixture of two triamines, one diamine, 2-formylpyridine and a ZnII salt was found to self-sort, cleanly producing a mixture of three different tetrahedral cages. Each cage bound one of three guests selectively. These guests could be released in a specific sequence following the addition of 4-methoxyaniline, which reacted with the cages, opening each in turn and releasing its guest. The system here described thus behaved in an organized way in three distinct contexts: cage formation, guest encapsulation, and guest release. Such behavior could be used in the context of a more complex system, WHERE released guests serve as signals to other chemical actors.	Mar 2014
I19-Small Molecule Single Crystal Diffraction	Empirical and theoretical insights into the structural features and host-guest chemistry of M8L4 tube architectures Wenjing Meng , Aaron B. League , Tanya K. Ronson , Jack K. Clegg , William C. Isley , David Semrouni , Laura Gagliardi , Christopher J. Cramer , Jonathan R. Nitschke Journal Of The American Chemical Society 136 (10) DOI: 10.1021/ja412964r Diamond Proposal Number(s): [7114, 7569] Show Abstract ▼ Abstract: We demonstrate a general method for the construction of M8L4 tubular complexes via subcomponent self-assembly, starting from CuI or AgI precursors together with suitable elongated tetraamine and 2-formylpyridine subcomponents. The tubular architectures were often observed as equilibrium mixtures of diastereomers having two different point symmetries (D2d or D2 ⇄ D4) in solution. The equilibria between diastereomers were influenced through variation in ligand length, substituents, metal ion identity, counteranion, and temperature. In the presence of dicyanoaurate(I) and AuI, the D4-symmetric hosts were able to bind linear Au(Au(CN)2)2– (with two different configurations) as the best-fitting guest. Substitution of dicyanoargentate(I) for dicyanoaurate(I) resulted in the formation of Ag(Au(CN)2)2– as the optimal guest through transmetalation. Density functional theory was employed to elucidate the host–guest chemistries of the tubes.	Jan 2014
I19-Small Molecule Single Crystal Diffraction	Bidirectional regulation of halide binding in a heterometallic supramolecular cube William Ramsay , Tanya Ronson , Jack Clegg , Jonathan R. Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.201307478 PMID: 24243650 Diamond Proposal Number(s): [7114, 7569] Show Abstract ▼ Abstract: Complex cubes: In a cationic supramolecular cube, coordinatively unsaturated metal centers in the walls of the host provided binding sites for neutral or negatively charged guests. The binding of an initial guest (CF3CO2−, OPMe3, NH3, or NMe3) either cooperatively enhanced or competitively inhibited the binding of a second guest (halide ion).	Nov 2013
I19-Small Molecule Single Crystal Diffraction	Chemical signals turn on guest binding through structural reconfiguration of triangular helicates Anne Sørensen , Ana M. Castilla , Tanya K. Ronson , Michael Pittelkow , Jonathan R. Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.201305245 PMID: 24038821 Diamond Proposal Number(s): [7984] Show Abstract ▼ Abstract: Be my guest: The function of a system based on self-assembled ZnII complexes can be controlled by external chemical stimuli. The complexes are based on a C3-symmetric ligand that forms a unique triangular triple helicate structure 1. Upon subcomponent substitution, 1 is able to transform into a triangular double helicate 2 which, unlike 1, can encapsulate guests.	Sep 2013
I19-Small Molecule Single Crystal Diffraction	A self-assembled [FeII12L12] capsule with an icosahedral framework Rana A. Bilbeisi , Tanya K. Ronson , Jonathan R. Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.201302976 PMID: 23857765 Diamond Proposal Number(s): [7569] Show Abstract ▼ Abstract: How about a different geometry? Depending on the reaction conditions, a threefold-symmetric triamine is observed to assemble into either the novel icosahedral [FeII12L12] capsule 1, or tetrahedral [FeII4L4] capsule 2. The two capsules have radically different cavity volumes and shapes, and are able to encapsulate guests of different size, shape, and charge.	Jul 2013
I19-Small Molecule Single Crystal Diffraction	Reactions of Cp2M (M = Ni, V) with dilithium diamido-aryl reagents; retention and oxidation of the transition metal ions Andrew E. H. Wheatley , Francesca A. Stokes , Mark A. Vincent , Ian H. Hillier , Tanya K. Ronson , Alexander Steiner , Paul T. Wood , Dominic S. Wright Dalton Transactions DOI: 10.1039/c3dt51632f Diamond Proposal Number(s): [7569] Open Access Show Abstract ▼ Abstract: The reactions of dilithium 1,2-diamidobenzene, [1,2-(HN)2C6H4]Li2 (L1H2)Li2, and dilithum 1,8-diamidonaphthalene, [1,8-(NH)2C10H6]Li2 (L2H2)Li2, with Cp2Ni and Cp2V have been used to obtain the new complexes (L2H2)2Ni{Li(THF)2}2 (3), (L2H2)3V{Li(THF)2}3 (4) and (L1H2)6Ni6.{[(L1H2)3(L1H)3Ni6Li(THF)]2.[Li(THF)4]+} (5), in which retention or oxidation of the initial metal(II) centre is observed. Whereas 3 and 4 contain one transition metal ion within ion-paired structures, 5 has a complicated co-crystalline composition which contains octahedral Ni6-cages constructed from six square-planar (16e) NiII centres.	Jul 2013
I19-Small Molecule Single Crystal Diffraction	Symmetry breaking in self-assembled M4L6 cage complexes Wenjing Meng , Tanya K. Ronson , Jonathan R. Nitschke Proceedings Of The National Academy Of Sciences DOI: 10.1073/pnas.1302683110 Diamond Proposal Number(s): [7569, 7114] Show Abstract ▼ Abstract: Here we describe the phenomenon of symmetry breaking within a series of M4L6 container molecules. These containers were synthesized using planar rigid bis-bidentate ligands based on 2,6-substituted naphthalene, anthracene, or anthraquinone spacers and FeII ions. The planarity of the ligand spacer favors a stereochemical configuration in which each cage contains two metal centers of opposite handedness to the other two, which would ordinarily result in an S4-symmetric, achiral configuration. Reduction of symmetry from S4 to C1 is achieved by the spatial offset between each ligand’s pair of binding sites, which breaks the S4 symmetry axis. Using larger CdII or CoII ions instead of FeII resulted, in some cases, in the observation of dynamic motion of the symmetry-breaking ligands in solution. NMR spectra of these dynamic complexes thus reflected apparent S4 symmetry owing to rapid interconversion between energetically degenerate, enantiomeric C1-symmetric conformations.	Jun 2013
I19-Small Molecule Single Crystal Diffraction	Chain-reaction anion exchange between metal–organic cages Shucong Ma , Maarten Marinus Johannes Smulders , Yana R. Hristova , Jack Clegg , Tanya Ronson , Salvatore Zarra , Jonathan R. Nitschke Journal Of The American Chemical Society 135 (15) DOI: 10.1021/ja311882h Diamond Proposal Number(s): [6791, 7114] Show Abstract ▼ Abstract: Differential binding affinities for a set of anions were observed between larger (1) and smaller (2) tetrahedral metal–organic capsules in solution. A chemical network could thus be designed wherein the addition of hexafluorophosphate could cause perchlorate to shift from capsule 2 to capsule 1 and triflimide to be ejected from capsule 1 into solution.	Mar 2013

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