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1.
Chemistry ; 26(22): 5093-5099, 2020 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-32065679

RESUMO

Understanding and controlling the topology of self-assembled structures plays a fundamental role in supramolecular chemistry. Herein, the preparation of a series of tetranuclear metallarectangles and hexanuclear trefoil knots featuring Cp*Rh building blocks by template-free self-assembly with four different rigid and flexible ligands is described. Transformations between the trefoil knots and the corresponding macrocycles can be induced by using concentration effects. Remarkably, the hexanuclear trefoil knot 5 was shown to assemble further to provide rare examples of [12+1] heteronuclear double trefoil knots (5 a/5 b/5 c/5 d) through coordination of the amide oxygen atoms to the secondary metal ions Na+ /K+ /Ca2+ /Cd2+ . The synthetic results are supported by single-crystal XRD.

2.
Nat Commun ; 10(1): 2057, 2019 05 03.
Artigo em Inglês | MEDLINE | ID: mdl-31053709

RESUMO

Over the past decades, molecular knots and links have captivated the chemical community due to their promising mimicry properties in molecular machines and biomolecules and are being realized with increasing frequency with small molecules. Herein, we describe how to utilize stacking interactions and hydrogen-bonding patterns to form trefoil knots, figure-eight knots and [2]catenanes. A transformation can occur between the unique trefoil knot and its isomeric boat-shaped tetranuclear macrocycle by the complementary concentration effect. Remarkably, the realization and authentication of the molecular figure-eight knot with four crossings fills the blank about 41 knot in knot tables. The [2]catenane topology is obtained because the selective naphthalenediimide (NDI)-based ligand, which can engender favorable aromatic donor-acceptor π interactions due to its planar, electron-deficient aromatic surface. The stacking interactions and hydrogen-bond interactions play important roles in these self-assembly processes. The advantages provide an avenue for the generation of structurally and topologically complex supramolecular architectures.

3.
Angew Chem Int Ed Engl ; 58(18): 5882-5886, 2019 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-30888717

RESUMO

A series of molecular metalla[2]catenanes featuring Cp*Ir vertices have been prepared by the template-free, coordination-driven self-assembly of dinuclear iridium acceptors and 1,5-bis[2-(4-pyridyl)ethynyl]anthracene donors. The metalla[2]catenanes were formed by using a strategically selected linker type that is capable of participating in sandwich-type π-π stacking interactions. In the solid state, the [2]catenanes adopt two different configurations depending on the halogen atoms at the dinuclear metal complex bridge. Altering the solvent or the concentration, as well as the addition of guest molecules, enabled controlled transformations between metalla[2]catenanes and tetranuclear metallarectangles.

4.
Dalton Trans ; 47(8): 2769-2777, 2018 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-29417108

RESUMO

Although reversible photo-dimerization or oxygenation of anthracene and its derivatives is a common reaction, light-initiated reversible conversion of endoperoxide organometallic frameworks has only rarely been addressed. Herein, a series of tetranuclear organometallic macrocycles, [Cp*2Rh2(µ-C2O4-κO)]2(BP4VA)2(OTf)4 (4), [Cp*2Rh2(BiBzIm)]2(BP4VA)2(OTf)4 (5), and [Cp*2Rh2(DHBQ)]2(BP4VA)2(OTf)4 (6), were obtained in good yields from the reactions of the binuclear half-sandwich rhodium precursors [Cp*2Rh2(µ-C2O4-κO)Cl2] (1), [Cp*2Rh2(BiBzIm)Cl2] (2), and [Cp*2Rh2(DHBQ)Cl2] (3) with the 9,10-bis((E)-2-(pyrid-4-yl)vinyl)anthracene (BP4VA) ligand. The photochemical reaction of these metallarectangles was investigated by NMR and UV/vis spectroscopy. We have demonstrated that complexes 4, 5, and 6 can be reversibly and nearly quantitatively converted to the macrocyclic endoperoxides 4-O2, 5-O2, and 6-O2. Meanwhile, the structure of the endoperoxide photoproducts was unambiguously confirmed by 1H/13C NMR spectroscopy, IR spectroscopy, elemental analyses, and X-ray crystallography.

5.
Dalton Trans ; 45(32): 12680-4, 2016 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-27476685

RESUMO

A Cp*Rh-based nonanuclear triangular macrocycle complex [(Cp*Rh)9L3(NO3)4.5(MeOH)](OTf)4.5 (1), a Cp*Ir-based trinuclear complex [(Cp*Ir)3L(MeCN)4](OTf)3 (2) and a linear heptanuclear heterometallic complex [(Cp*Ir)6ZnL2(MeCN)8(MeOH)2](OTf)8 (3) (Cp* = η(5)-pentamethylcyclopentadienyl) have been synthesized from a 2-(4-(pyridin-4-yl)phenyl)-1H-imidazole-4,5-dicarboxylic acid proligand. These complexes were further characterized by X-ray crystallography, (1)H NMR, DOSY NMR, IR spectroscopy, and elemental analyses.

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