A metallo-supramolecular double-helix containing a major and a minor groove

Hannon, Michael J.; Painting, Claire L.; Alcock, Nathaniel W.

doi:10.1039/a905795a

Cited by 132 publications

(68 citation statements)

References 8 publications

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“…In particular, we have developed an "inexpensive approach" to generate sophisticated supramolecular architectures based on the interaction of metal ions with imine-based ligands [9][10][11][12]. Of particular importance to this work, a synthetic procedure has been described for making a tetracationic supramolecular cylinders with a triple helical architecture ( Fig.…”

Section: Introductionmentioning

confidence: 99%

Interaction between a DNA oligonucleotide and a dinuclear iron(II) supramolecular cylinder; an NMR and molecular dynamics study

et al. 2002

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Section: Introductionmentioning

confidence: 99%

Interaction between a DNA oligonucleotide and a dinuclear iron(II) supramolecular cylinder; an NMR and molecular dynamics study

et al. 2002

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“…In addition to the metal-ligand interactions, which drive the formation, the structure is stabilized via interstrand face-edge -stacking interactions between the phenylene rings of the spacer groups. If the ligands are reacted with tetrahedral metal ions, such as Cu I and Ag I , dinuclear double-stranded cations [M 2 L 2 ] 2ϩ are produced [28,29]. These dinuclear double-stranded species exists in two conformations: a double helix (rac-isomer) and a box structure (meso-isomer), with the latter favored at low temperatures.…”

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confidence: 99%

Electron capture dissociation mass spectrometry of metallo-supramolecular complexes

Kaczorowska

Hotze

Hannon

et al. 2010

J. Am. Soc. Mass Spectrom.

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The electron capture dissociation (ECD) of metallo-supramolecular dinuclear triple-stranded helicate Fe 2 L 3 4ϩ ions was determined by Fourier transform ion cyclotron resonance mass spectrometry. Initial electron capture by the di-iron(II) triple helicate ions produces dinuclear double-stranded complexes analogous to those seen in solution with the monocationic metal centers Cu I or Ag I . The gas-phase fragmentation behavior [ECD, collision-induced dissociation (CID), and infrared multiphoton dissociation (IRMPD)] of the di-iron double-stranded complexes, (i.e., MS 3 of the ECD product) was compared with the ECD, CID, and IRMPD of the Cu I and Ag I complexes generated from solution. The results suggest that iron-bound dimers may be of the form Fe I 2 L 2 2ϩ and that ECD by metallo-complexes allows access, in the gas phase, to oxidation states and coordination chemistry that cannot be accessed in solution. (J Am Soc Mass Spectrom 2010, 21, 300 -309) © 2010 American Society for Mass Spectrometry T he benefits of mass spectrometry in the study of supramolecular chemistry are several: investigation of molecules and complexes in the gas phase allows determination of the intrinsic properties without interference from solvent or counter ion [1]. Comparison of gas-and condensed-phase behavior provides information on solvation effects. While most applications of MS to supramolecular assemblies focus on soft ionization techniques, e.g., coldspray [2] and desorption electrospray ionization (DESI) [3], to retain the assembly intact, structural information can be gained by tandem mass spectrometry (MS/MS) in which precursor ions are characterized according to their fragment ions. It is also possible to obtain information regarding fundamental reactivity by MS/MS. To date, MS/MS techniques applied to supramolecular chemistry include collision-induced dissociation (CID) to obtain structural information [4], infrared multiphoton dissociation (IRMPD) for the study of reactivity and mechanisms of fragmentation in the gas phase [5][6][7], and blackbody infrared radiation dissociation (BIRD) for the study of gas-phase kinetics [8].Here, we have applied electron capture dissociation (ECD) to the study of metallo-supramolecular doubleand triple-stranded helicates. Electron capture dissociation (ECD) [9,10] is a relatively recent tandem mass spectrometry technique in which trapped ions are irradiated with low-energy electrons provided by a heated dispenser cathode [11]. (The requirement for trapped ions and electrons means that ECD is generally only performed in a Fourier transform ion cyclotron resonance (FT-ICR) [12] mass spectrometer). As with other recent technological advances in mass spectrometry, the development of ECD has been driven by its application to biosciences, particularly in the analysis of peptides and proteins, although the technique has recently been applied to some synthetic macromolecules, such as polymers and dendrimers [13][14][15][16][17][18][19]. The ECD of metalbound peptide [20 -23] and lipid complexes [...

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“…Furthermore, Williams, [77,78] Hannon, [58,60] and Yoshida [62,63] and their respective co-workers already introduced the methylene-bridged ligands 6 and 7, which form the triple-stranded homochiral helicates [ (6) NMR investigation of the diamagnetic triple-stranded helicate [(7 a) 3 Fe 2 ] 4 + shows that this chiral complex is formed in a highly diastereoselective way. [58,60] The corresponding dinuclear zinc complex [(7 a) 3 Zn 2 ]…”

Section: Discussionmentioning

confidence: 98%

Long‐Range Stereocontrol in the Self‐Assembly of Two‐Nanometer‐Dimensioned Triple‐Stranded Dinuclear Helicates

Albrecht¹,

Janser²,

Houjou³

et al. 2004

Chemistry A European J

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A series of bisimine-bridged dicatechol ligands 2-H(4)-5-H(4) were synthesized and were used to prepare triple-stranded dinuclear helicate-type complexes with a length of up to more than 2 nm. X-ray structural analyses of Na(4)[(2)(3)V(2)], Na(4)[(3)(3)Ti(2)], Na(4)[(4)(3)Ti(2)], and Na(4)[(5)(3)Ti(2)], as well as temperature-dependent NMR investigations of Na(4)[(4)(3)Ti(2)] and Na(4)[(5)(3)Ti(2)] show that, in the case of the rigid linear ligands 2 and 3, and of the ligand 5, which possesses C(2h) symmetry in its idealized structure, homochiral helicates are diastereoselectively formed. Ligand 4, on the other hand, with idealized C(2v) symmetry, leads with surprisingly high selectivity to the formation of the heterochiral meso-helicate. This is attributed to the ability of ligand 4 to adopt a less-restricted conformation in the meso compound than in the helical complex. NMR investigations indicate that both complex units of Na(4)[(4)(3)Ti(2)] invert (LambdaDelta-->DeltaLambda) simultaneously, while in the case of Na(4)[(5)(3)Ti(2)] a stepwise racemization proceeds.

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A metallo-supramolecular double-helix containing a major and a minor groove

Cited by 132 publications

References 8 publications

Interaction between a DNA oligonucleotide and a dinuclear iron(II) supramolecular cylinder; an NMR and molecular dynamics study

Interaction between a DNA oligonucleotide and a dinuclear iron(II) supramolecular cylinder; an NMR and molecular dynamics study

Electron capture dissociation mass spectrometry of metallo-supramolecular complexes

Long‐Range Stereocontrol in the Self‐Assembly of Two‐Nanometer‐Dimensioned Triple‐Stranded Dinuclear Helicates

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