New Three-Fold Interpenetrated Uranyl Organic Framework Constructed by Terephthalic Acid and Imidazole Derivative

Chen, Fei; Wang, Cong-zhi; Li, Zi‐Jie; Lan, Jian‐Hui; Ji, Yanqin; Chai, Zhifang

doi:10.1021/acs.inorgchem.5b00013

Cited by 38 publications

(33 citation statements)

References 42 publications

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“…Recently,o ur group reported ar are case of an onlinear[ O =U=O] bond with ab ond angle of 173.3(5)8 in au ranyl complex with terephthalica cid and bis-imidazole ligands. [20] Here, the bond angle of 172.0(9)8 represents am ore significant bending of the [O=U=O] bond, which might result in al arger extent of inert U=Oa ctivation. [21] The unique trinuclearu ranyl units in at ridentate mode offer a2 Dp olyrotaxane network, whereas the sulfate ion-bridged uranyl dimers extendi nto a1 Dp olyrotaxanec hain in compound 1.These two isolated supramolecular polyrotaxane moi-eties can further interact with each other,w here different layers of 2D polyrotaxane networks are threaded in an ordered array of 1D polyrotaxane chains (Figures 4a-d andS 8i nt he Supporting Information).…”

Section: Synthesis and Crystallographic Analysis Of Compoundmentioning

confidence: 99%

An Unprecedented Two‐Fold Nested Super‐Polyrotaxane: Sulfate‐Directed Hierarchical Polythreading Assembly of Uranyl Polyrotaxane Moieties

Mei

Yuan

et al. 2016

Chemistry A European J

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The hierarchical assembly of well-organized submoieties could lead to more complicated superstructures with intriguing properties. We describe herein an unprecedented polyrotaxane polythreading framework containing a two-fold nested super-polyrotaxane substructure, which was synthesized through a uranyl-directed hierarchical polythreading assembly of one-dimensional polyrotaxane chains and two-dimensional polyrotaxane networks. This special assembly mode actually affords a new way of supramolecular chemistry instead of covalently linked bulky stoppers to construct stable interlocked rotaxane moieties. An investigation of the synthesis condition shows that sulfate can assume a vital role in mediating the formation of different uranyl species, especially the unique trinuclear uranyl moiety [(UO2 )3 O(OH)2 ](2+) , involving a notable bent [O=U=O] bond with a bond angle of 172.0(9)°. Detailed analysis of the coordination features, the thermal stability as well as a fluorescence, and electrochemical characterization demonstrate that the uniqueness of this super-polyrotaxane structure is mainly closely related to the trinuclear uranyl moiety, which is confirmed by quantum chemical calculations.

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Section: Synthesis and Crystallographic Analysis Of Compoundmentioning

confidence: 99%

An Unprecedented Two‐Fold Nested Super‐Polyrotaxane: Sulfate‐Directed Hierarchical Polythreading Assembly of Uranyl Polyrotaxane Moieties

Mei

Yuan

et al. 2016

Chemistry A European J

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“…4,5 Although our studies of complexes of cis-1,2-cyclohexanedicarboxylate have to date been limited, they do indicate significant differences to be associated with this isomeric form, providing reason for an extension to examination of the complexes of cis-and trans-1,4-cyclohexanedicarboxylic acid, for which but a single uranyl molecular complex of the trans isomer is known. 6 This acid is the alicyclic counterpart of terephthalic acid, which has been used in the synthesis of several coordination polymers, [7][8][9][10][11][12][13][14][15][16][17][18][19] most often one-or two-dimensional (1D or 2D), with only two cases of threedimensional (3D) frameworks, 12,16 and also some examples of interpenetrated nets. 8,14,19 Some of these complexes are heterometallic, 7,11,13,18 and display photocatalytic activity.…”

Section: Introductionmentioning

confidence: 99%

“…6 This acid is the alicyclic counterpart of terephthalic acid, which has been used in the synthesis of several coordination polymers, [7][8][9][10][11][12][13][14][15][16][17][18][19] most often one-or two-dimensional (1D or 2D), with only two cases of threedimensional (3D) frameworks, 12,16 and also some examples of interpenetrated nets. 8,14,19 Some of these complexes are heterometallic, 7,11,13,18 and display photocatalytic activity. 7,13,18 We used two commercially available forms of 1,4-cyclohexanedicarboxylic acid, the pure trans form (t-1,4-chdcH2), which, when the two acid groups are in equatorial position, is geometrically close to terephthalic acid, and a mixture of cis and trans isomers (c,t-1,4-chdcH2).…”

Section: Introductionmentioning

confidence: 99%

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Structural Consequences of 1,4-Cyclohexanedicarboxylate Cis/Trans Isomerism in Uranyl Ion Complexes: From Molecular Species to 2D and 3D Entangled Nets

2017

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trans-1,4-Cyclohexanedicarboxylic acid (t-1,4-chdcH) or the commercially available mixture of the cis and trans isomers (c,t-1,4-chdcH) has been used in the synthesis of a series of 14 uranyl ion complexes, all obtained under solvohydrothermal conditions, some in the presence of additional metal cations and/or 2,2'-bipyridine (bipy). With its two isomeric forms having very different shapes and its great sensitivity to the experimental conditions, 1,4-chdc appears to be suitable for the synthesis of uranyl ion complexes displaying a wide range of architectures. Under the conditions used, the pure trans isomer gives only the complexes [UO(t-1,4-chdc)(HO)] (1) and [UO(t-1,4-chdc)] (2), which crystallize as one- and two-dimensional (1D and 2D) species, respectively. Complexes containing either the cis isomer alone or mixtures of the two isomers in varying proportion were obtained from the isomer mixture. The neutral complexes [UO(c-1,4-chdc)(DMF)] (3) and [UO(c-1,4-chdc)(bipy)] (4) are 2D and 1D assemblies, respectively, while all the other complexes are anionic and include various counterions. [C(NH)][HNMe][(UO)(c-1,4-chdc)]·HO (5) crystallizes as a three-dimensional (3D) framework with {10} topology. While [HNMe][(UO)(c-1,4-chdc)(t-1,4-chdc)]·DMF·2HO (6) is a 1D ladderlike polymer, [HNMe][(UO)(c-1,4-chdc)(t-1,4-chdc)]·2HO (7), which differs in the cis/trans ratio, is a 3-fold 2D interpenetrated network with {6} honeycomb topology. The related [HNMe][(UO)(c,t-1,4-chdc)]·2.5HO (8), with one disordered ligand of uncertain geometry, is a 3-fold 3D interpenetrated system. The two isomorphous complexes [Co(bipy)][(UO)(c-1,4-chdc)]·1.5HO (9) and [Cd(bipy)][(UO)(c-1,4-chdc)]·1.5HO (10) form 3D frameworks with the {10} srs topological type. In contrast, [Ni(bipy)][(UO)(c-1,4-chdc)(t-1,4-chdc)(NO)]·2HO (11) is a molecular, tetranuclear complex due to the presence of terminal nitrate ligands. A 2-fold 3D interpenetration of frameworks with {10} ths topology is observed in [Cu(bipy)][(UO)(c-1,4-chdc)(t-1,4-chdc)]·2HO (12), while [Zn(bipy)][(UO)(c-1,4-chdc)]·4HO (13) crystallizes as a 2D net with the common {4.8} fes topological type. The additional Pb cation is an essential part of the 3D framework formed in [UOPb(c-1,4-chdc)(t-1,4-chdc)(bipy)] (14), in which uranyl and its ligands alone form 1D subunits. Together with previous results, the solid-state uranyl emission properties of seven of the present complexes evidence a general trend, with the maxima for the complexes with O equatorial environments being blue-shifted with respect to those for complexes with O environments.

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“…[1,9] In metallasupramolecular chemistry, although the pyridine-based ligands have been widely used as rigid neutral bridging linkers, the use of the imidazole-based linkers is still limited. Jin, [10] Mukherjee [11] and others [12] have reported several imidazole-based bridging ligands which are similar to pyridine-based ligands. They have also demonstrated that the imidazole-derivatives can bind metal ions much stronger than pyridyl linkers.…”

Section: Introductionmentioning

confidence: 96%

Incorporation of Core‐Twisted Perylene Bisimide Ligands into a Discrete Cp*Rh‐Based Molecular‐Rectangle via Coordination‐Driven Self‐Assembly

Zhang

Das

Han

2019

Israel Journal of Chemistry

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A tetranuclear metallarectangle (2) derived from dinuclear rhodium(III) building block [Cp*2Rh2(μ‐η2‐η2‐C2O4)]Cl2 and imidazole‐based perylene bisimide ditopic ligand (1) (1=2,9‐bis(4‐(1H‐imidazol‐1‐yl)phenyl)‐5,6,12,13‐tetrachloroanthra‐[2,1,9‐def:6,5,10‐d′e′f′]diisoquinoline‐1,3,8,10(2H,9H)‐tetraone) in presence of silver triflate is reported. The self‐assembled metallarectangle 2 is fully characterized by NMR, ESI‐MS, UV‐vis absorption, fluorescence emission spectroscopy and cyclic voltammetry. The X‐ray diffraction analysis reveals a twisted conformational geometry of metallarectangle 2 caused by essential steric demands of the two side‐by‐side chlorine atoms. In addition, the analyzed structure also elaborates the intermolecular electrostatic interactions between the electron‐deficient diimide moiety of 2 and the electron‐rich planar phenanthrene molecule.

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New Three-Fold Interpenetrated Uranyl Organic Framework Constructed by Terephthalic Acid and Imidazole Derivative

Cited by 38 publications

References 42 publications

An Unprecedented Two‐Fold Nested Super‐Polyrotaxane: Sulfate‐Directed Hierarchical Polythreading Assembly of Uranyl Polyrotaxane Moieties

An Unprecedented Two‐Fold Nested Super‐Polyrotaxane: Sulfate‐Directed Hierarchical Polythreading Assembly of Uranyl Polyrotaxane Moieties

Structural Consequences of 1,4-Cyclohexanedicarboxylate Cis/Trans Isomerism in Uranyl Ion Complexes: From Molecular Species to 2D and 3D Entangled Nets

Incorporation of Core‐Twisted Perylene Bisimide Ligands into a Discrete Cp*Rh‐Based Molecular‐Rectangle via Coordination‐Driven Self‐Assembly

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