The first case of actinide triple helices: pH-dependent structural evolution and kinetically-controlled transformation of two supramolecular conformational isomers

An, Shu‐wen; Mei, Lei; Wang, Cong-zhi; Xia, Chuanqin; Chai, Zhifang

doi:10.1039/c5cc02646f

Cited by 39 publications

(36 citation statements)

References 40 publications

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“…As shown in Figure a, the U1 ion has an almost ideal hexagonal bipyramidal coordination environment defined by six oxygen atoms from three MTB 4− ligands (the U−O bond distances range from 2.455(5) to 2.470(5) Å) in the equatorial plane and two acyl oxygen atoms (the O3=U=O4 angle is 180.00(19)°, and the U=O distances are 1.692(8) and 1.713(9) Å) at the axial positions, respectively (Supporting Information, Table S2). All the angles and bond distances are in good agreement with relevant parameters reported previously . As shown in the Supporting Information, Figure S9a and S10, the shortest loop of 1 consists of four MTB 4− ligands and four uranyl cations.…”

Section: Figuresupporting

confidence: 88%

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Solvent‐Dependent Synthesis of Porous Anionic Uranyl–Organic Frameworks Featuring a Highly Symmetrical (3,4)‐Connected ctn or bor Topology for Selective Dye Adsorption

Jiang²,

Wang

et al. 2016

Chemistry A European J

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Two highly symmetrical (3,4)-connected uranyl-organic frameworks (UOFs) were synthesized by a judicious combination of D -symmetrical triangular [UO (COO) ] and T symmetrical tetrahedral tetrakis(4-carboxyphenyl)methane (H MTB). These two as-synthesized UOFs possess similar structural units and coordination modes but totally different topological structures, namely ctn net and bor net. Solvent-induced interpenetration and a morphology change are observed. The two compounds exhibit crystal transformation via a dissolution-crystallization process. Adsorption experiments in CH OH solution indicate that both of them can selectively remove positively charged dyes over negatively charged and neutral dyes. Moreover, the electronic structural and bonding properties of the two compounds were systematically explored by density functional theory (DFT) calculations.

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Section: Figuresupporting

confidence: 88%

“…Similarly, crystal samples of 1 can also be obtained via the reaction of 2 in DMF. Taking into account the failure of crystal transformation in the solid state, it is reasonable to believe that a dissolution–crystallization process should be involved in the crystal transformation …”

Section: Figurementioning

confidence: 99%

Solvent‐Dependent Synthesis of Porous Anionic Uranyl–Organic Frameworks Featuring a Highly Symmetrical (3,4)‐Connected ctn or bor Topology for Selective Dye Adsorption

Jiang²,

Wang

et al. 2016

Chemistry A European J

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“…The inactive terminal oxo groups of uranyl often prevent axial bonding interactions, resulting in any further coordination occurring in the equatorial plane. As a result, uranyl-organic coordination polymers usually prefer to form onedimensional (1D) chains, 10,[15][16][17] or two-dimensional (2D) sheets, [18][19][20][21][22][23][24] rather than threedimensional (3D) frameworks that require structural connectivity in the third axial dimension. [25][26][27][28][29][30][31][32] 2D networks or 3D frameworks with large cavities or pores can readily achieve a high degree of self-assembly by an entangled mode in the solid state, and thus afford a variety of intriguing topological structures as well as fascinating properties.…”

Section:  Introductionmentioning

confidence: 99%

Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks

Mei¹,

Wang²,

Zhu³

et al. 2017

Inorg. Chem.

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The reaction of uranyl nitrate with terephthalic acid (HTP) under hydrothermal conditions in the presence of an organic base, 1,3-(4,4'-bispyridyl)propane (BPP) or 4,4'-bipyridine (BPY), provided four uranyl terephthalate compounds with different entangled structures by a pH-tuning method. [UO(TP)](HBPP)·2HO (1) obtained in a relatively acidic solution (final aqueous pH, 4.28) crystallizes in the form of a noninterpenetrated honeycomb-like two-dimensional network structure. An elevation of the solution pH (final pH, 5.21) promotes the formation of a dimeric uranyl-mediated polycatenated framework, [(UO)(μ-OH)(TP)](HBPP)·4.5HO (2). Another new polycatenated framework with a monomeric uranyl unit, [(UO)(TP)](HBPP) (3), begins to emerge as a minor accompanying product of 2 when the pH is increased up to 6.61, and turns out to be a significant product at pH 7.00. When more rigid but small-size BPY molecules replace BPP molecules, [UO(TP)](HBPP) (4) with a polycatenated framework similar to 3 was obtained in a relatively acidic solution (final pH, 4.81). The successful preparation of 2-4 represents the first report of uranyl-organic polycatenated frameworks derived from a simple HTP linker. A direct comparison between these polycatenated frameworks and previously reported uranyl terephthalate compounds suggests that the template and cavity-filling effects of organic bases (such as BPP or BPY), in combination with specific hydrothermal conditions, promote the formation of uranyl terephthalate polycatenated frameworks.

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“…Polypyridyl chelating N‐donors feature relatively large binding affinities for f‐element ions (specifically the [UO 2 ] 2+ cation) 36. Some of the ligands of this class, such as 1,10‐phenanthroline (phen) and 2,2′:6′,2″‐terpyridine (terpy) (and its derivatives), have been explored as “capping” ligands in the synthesis uranyl coordination polymers,18,37–40 molecular uranyl materials,41–44 and lanthanide hybrid materials 45–47. Herein we are using these ligands explicitly as tools for crystal engineering by the chelation of part of the equatorial uranyl coordination sphere, thus promoting further assembly by halogen or hydrogen bonding, π–π stacking interactions, or a combination thereof.…”

Section: Introductionmentioning

confidence: 99%

Probing the Influence of N‐Donor Capping Ligands on Supramolecular Assembly in Molecular Uranyl Materials

2015

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The syntheses and crystal structures of six new compounds containing the UO 2 2+ cation, 3,5-dichlorobenzoic acid, and a chelating N-donor [2,2′-bipyridine (bipy), 1,10-phenanthroline (phen), 4,7-dimethyl-1,10-phenanthroline (dimethylphen), 2,2′:6′,2′′-terpyridine (terpy), 4′-chloro-2,2′:6′,2′′-terpyridine (Cl-terpy), or 2,4,6-tris(2-pyridyl)-s-triazine (TPTZ)] are reported. Single-crystal X-ray diffraction analysis of these materials enabled the exploration of the structural relationship between the benzoic acids and the chelating N-donor as well as providing a platform to evaluate the effects of ligand choice on uranyl hydrolysis and subsequent oligomerization. At an unadjusted pH (ca. 3), a mix of uranyl monomers and dimers are [a] All organic materials, 3,5-dichlorobenzoic acid (Alfa Aesar, 99 %) and the chelating N-donors [2,2′-bipyridine (Sigma Aldrich, 99+%), 1,10-Eur. J. Inorg. Chem. 2016, 126-137 www.eurjic.org Eur. J. Inorg. Chem. 2016, 126-137 www.eurjic.org136 order to increase the sample concentration and enhance the resulting luminescence spectra. The solid material was then allowed to air-dry for approximately ten minutes, allowing for the evaporation of the cyclohexane, and then a cover slide was placed on top of the sample and secured with adhesive tape.Supporting Information (see footnote on the first page of this article): ORTEP figures of all compounds, PXRD spectra of all compounds, IR spectra of complexes 1, 4, and 5, and tables of selected supramolecular interaction distances and bond lengths are all available. Note:The authors declare no competing financial interest.

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The first case of actinide triple helices: pH-dependent structural evolution and kinetically-controlled transformation of two supramolecular conformational isomers

Cited by 39 publications

References 40 publications

Solvent‐Dependent Synthesis of Porous Anionic Uranyl–Organic Frameworks Featuring a Highly Symmetrical (3,4)‐Connected ctn or bor Topology for Selective Dye Adsorption

Solvent‐Dependent Synthesis of Porous Anionic Uranyl–Organic Frameworks Featuring a Highly Symmetrical (3,4)‐Connected ctn or bor Topology for Selective Dye Adsorption

Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks

Probing the Influence of N‐Donor Capping Ligands on Supramolecular Assembly in Molecular Uranyl Materials

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