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Title: Synthesis, structure, luminescence and photocatalytic properties of an uranyl-2,5-pyridinedicarboxylate coordination polymer

Abstract

An uranium coordination polymer, namely [(UO{sub 2}(pydc)(H{sub 2}O)]·H{sub 2}O (1) (H{sub 2}pydc=2,5-pyridinedicarboxylic acid), has been obtained by hydrothermal method and characterized by X-ray single crystal structure determination. Structural analysis reveals that complex 1 exhibits 1D chain coordination polymer, in which UO{sub 2}{sup 2+} ions are bridged by 2,5-pyridinedicarboxylate ligands and the chains are connected into a 3D supramolecular network by O–H···O hydrogen bond interactions and π–π stacking interactions. The photocatalytic properties of 1 for degradation of methylene blue (MB), Rhodamine B (RhB) and methyl orange (MO) under Hg-lamp irradiation have been performed, and the amount of the catalyst as well as Hg-lamp irradiation with different power on the photodegradation efficiency of MB have been investigated. Elemental analyses, infrared spectroscopy, TG-DTA analyses and luminescence properties were also discussed. - Graphical abstract: Complex 1 exhibits 1D chain coordination polymer in which UO{sub 2}{sup 2+} ions are bridged by 2,5-pyridinedicarboxylate ligand. Photoluminescence studies reveal that complex 1 exhibits characteristic emissions of uranyl centers. The compound is selective to degraded dye and displays good photocatalytic activities for the degradation of MB under Hg-lamp. Display Omitted - Highlights: • Complex 1 exhibits 1D chain coordination polymer. • Complex 1 could degrade methylene blue and Rhodaminemore » B under Hg-lamp irradiation. • Luminescent property of 1 has been studied.« less

Authors:
; ;
Publication Date:
OSTI Identifier:
22584154
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Solid State Chemistry; Journal Volume: 239; Other Information: Copyright (c) 2016 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION SPECTROSCOPY; CATALYSTS; CRYSTAL STRUCTURE; DIFFERENTIAL THERMAL ANALYSIS; HYDROTHERMAL SYNTHESIS; INFRARED SPECTRA; INTERACTIONS; IONS; IRRADIATION; LIGANDS; METHYL ORANGE; METHYLENE BLUE; MONOCRYSTALS; PHOTOCATALYSIS; PHOTOLUMINESCENCE; POLYMERS; RHODAMINES; URANIUM DIOXIDE; WATER; X RADIATION

Citation Formats

Si, Zhen-Xiu, Xu, Wei, E-mail: xuwei@nbu.edu.cn, and Zheng, Yue-Qing, E-mail: yqzhengmc@163.com. Synthesis, structure, luminescence and photocatalytic properties of an uranyl-2,5-pyridinedicarboxylate coordination polymer. United States: N. p., 2016. Web. doi:10.1016/J.JSSC.2016.04.024.
Si, Zhen-Xiu, Xu, Wei, E-mail: xuwei@nbu.edu.cn, & Zheng, Yue-Qing, E-mail: yqzhengmc@163.com. Synthesis, structure, luminescence and photocatalytic properties of an uranyl-2,5-pyridinedicarboxylate coordination polymer. United States. doi:10.1016/J.JSSC.2016.04.024.
Si, Zhen-Xiu, Xu, Wei, E-mail: xuwei@nbu.edu.cn, and Zheng, Yue-Qing, E-mail: yqzhengmc@163.com. 2016. "Synthesis, structure, luminescence and photocatalytic properties of an uranyl-2,5-pyridinedicarboxylate coordination polymer". United States. doi:10.1016/J.JSSC.2016.04.024.
@article{osti_22584154,
title = {Synthesis, structure, luminescence and photocatalytic properties of an uranyl-2,5-pyridinedicarboxylate coordination polymer},
author = {Si, Zhen-Xiu and Xu, Wei, E-mail: xuwei@nbu.edu.cn and Zheng, Yue-Qing, E-mail: yqzhengmc@163.com},
abstractNote = {An uranium coordination polymer, namely [(UO{sub 2}(pydc)(H{sub 2}O)]·H{sub 2}O (1) (H{sub 2}pydc=2,5-pyridinedicarboxylic acid), has been obtained by hydrothermal method and characterized by X-ray single crystal structure determination. Structural analysis reveals that complex 1 exhibits 1D chain coordination polymer, in which UO{sub 2}{sup 2+} ions are bridged by 2,5-pyridinedicarboxylate ligands and the chains are connected into a 3D supramolecular network by O–H···O hydrogen bond interactions and π–π stacking interactions. The photocatalytic properties of 1 for degradation of methylene blue (MB), Rhodamine B (RhB) and methyl orange (MO) under Hg-lamp irradiation have been performed, and the amount of the catalyst as well as Hg-lamp irradiation with different power on the photodegradation efficiency of MB have been investigated. Elemental analyses, infrared spectroscopy, TG-DTA analyses and luminescence properties were also discussed. - Graphical abstract: Complex 1 exhibits 1D chain coordination polymer in which UO{sub 2}{sup 2+} ions are bridged by 2,5-pyridinedicarboxylate ligand. Photoluminescence studies reveal that complex 1 exhibits characteristic emissions of uranyl centers. The compound is selective to degraded dye and displays good photocatalytic activities for the degradation of MB under Hg-lamp. Display Omitted - Highlights: • Complex 1 exhibits 1D chain coordination polymer. • Complex 1 could degrade methylene blue and Rhodamine B under Hg-lamp irradiation. • Luminescent property of 1 has been studied.},
doi = {10.1016/J.JSSC.2016.04.024},
journal = {Journal of Solid State Chemistry},
number = ,
volume = 239,
place = {United States},
year = 2016,
month = 7
}
  • The hydrothermal reactions of MnCl{sub 2}.4H{sub 2}O, 3,4-pyridinedicarboxylic acid (3,4-pydaH{sub 2}) and triethylamine in aqueous medium yield two 3D metal-organic hybrid materials, [Mn(3,4-pyda)] (1) and [Mn{sub 3}(OH){sub 2}(3,4-pyda){sub 2}(H{sub 2}O){sub 2}] (2), respectively. In both complexes, each 3,4-pyda acts as a pentadentate ligand to connect five Mn(II) atoms via the pyridyl group and the two {mu}{sub 2}-carboxylate groups (one in syn,anti-mode and one in syn-syn mode for 1 and both in syn,anti-mode for 2). Complex 1 possesses an interesting 3D coordination polymeric structure incorporating 1D helical Mn({mu}{sub 2}-carboxylate){sub 2} chain units, in which each Mn(II) atom is coordinated in lessmore » common square pyramidal geometry to four carboxylato oxygen atoms and one pyridyl nitrogen atom. Each 3,4-pyda links three helical Mn({mu}{sub 2}-carboxylate){sub 2} chains and each Mn({mu}{sub 2}-carboxylate){sub 2} chain is linked by other eight helical Mn({mu}{sub 2}-carboxylate){sub 2} chains via sharing 3,4-pyda bridges. Complex 2 is a 3D coordination network consisting of 1D Mn{sub 3}(OH){sub 2} chains and 3,4-pyda bridges. The repeating trimeric structural unit in the manganese(II) hydroxide chain consists of two edge-sharing symmetry-related manganese octahedra linked via {mu}{sub 3}-OH to a vertex of Mn{sub 2} octahedron. Each 3,4-pyda links three Mn{sub 3}(OH){sub 2} chains and each Mn{sub 3}(OH){sub 2} chain is linked by other six Mn{sub 3}(OH){sub 2} chains via 3,4-pyda bridges, resulting in a 3D coordination solid. Magnetic measurements reveal that a weak antiferromagnetic interaction between the Mn{sup II} ions occurs in complex 1 and a 3D magnetic ordering at about 7.0K in complex 2.« less
  • Reaction of Ln(NO{sub 3}){sub 3}.6H{sub 2}O with H{sub 2}L [H{sub 2}L=N,N'-bis(salicylidene)propane-1,2-diamine] gives rise to five new coordination polymers, viz. [Pr(H{sub 2}L)(NO{sub 3}){sub 3}(MeOH)]{sub n} (1) and [Ln(H{sub 2}L){sub 1.5}(NO{sub 3}){sub 3}]{sub n} [Ln=La (2), Eu (3), Sm (4) and Gd (5)]. Crystal structural analysis reveals that H{sub 2}L effectively functions as a bridging ligand forming one-dimensional (1D) chain and two-dimensional (2D) open-framework polymers. Solid-state fluorescence spectra of 3 and 4 exhibit typical red fluorescence of Eu(III) and Sm(III) ions at room temperature while 2 emits blue fluorescence of ligand H{sub 2}L. The lowest triplet level of ligand H{sub 2}L wasmore » calculated on the basis of the phosphorescence spectrum of 5. The energy transfer mechanisms in the lanthanide polymers were described and discussed. - Graphical abstract: Five coordination polymers were synthesized. Given is the perspective view of a H{sub 2}L bridged hexametal ring along the c axis for 2 (La), excitation and emission spectra of 3 (Eu) and 4 (Sm) in the solid state.« less
  • Two new lanthanide coordination polymers based on a semirigid bridging thenylsalicylamide ligand ([Ln{sub 2}L{sub 3}(NO{sub 3}){sub 6}]·(C{sub 4}H{sub 8}O{sub 2}){sub 2}){sub ∞} were obtained and characterized by elemental analysis, X-ray diffraction, IR and TGA measurements. The two compounds are isostructure and possess one dimensional trapezoid ladder-like chain built up from the connection of isolated LnO{sub 3}(NO{sub 3}){sub 3} polyhedra (distorted monocapped antisquare prism) through the ligand. The photoluminescence analysis suggest that there is an efficient ligand-to-Ln(III) energy transfer in Tb(III) complex and the ligand is an efficient “antenna” for Tb(III). From a more general perspective, the results demonstrated herein providemore » the possibility of controlling the formation of the desired lanthanide coordination structure to enrich the crystal engineering strategy and enlarge the arsenal for developing excellent luminescent lanthanide coordination polymers. - Graphical abstract: We present herein one dimensional lanthanide coordination polymers of a new semirigid exo-bidentate ligand which not only display interesting structures but also possess strong luminescence properties. Display Omitted - Highlights: • We present lanthanide coordination polymers of a new semirigid exo-bidentate ligand. • The lanthanide coordination polymers exhibit interesting structures. • The luminescent properties of Tb(III) complexes are discussed in detail.« less
  • The new semirigid exo-bidentate ligand incorporating furfurysalicylamide terminal groups, namely, 1,4-bis([(2′-furfurylaminoformyl)phenoxyl]methyl)-2,5-bismethylbenzene (L) was synthesized and used as building blocks for constructing lanthanide coordination polymers with luminescent properties. The series of lanthanide nitrate complexes have been characterized by elemental analysis, IR spectroscopy, and X-ray diffraction analysis. The semirigid ligand L, as a bridging ligand, reacts with lanthanide nitrates forming three distinct structure types: chiral noninterpenetrated two-dimensional (2D) honeycomblike (6,3) (hcb, Schläfli symbol 6{sup 3}, vertex symbol 6 6 6) topological network as type I, 1D zigzag chain as type II and 1D trapezoid ladder-like chain as type III. The structural diversitiesmore » indicate that lanthanide contraction effect played significant roles in the structural self-assembled process. The luminescent properties of Eu{sup III}, Tb{sup III} and Dy{sup III} complexes are discussed in detail. Due to the good match between the lowest triplet state of the ligand and the resonant energy level of the lanthanide ion, the lanthanide ions in Eu{sup III}, Tb{sup III} and Dy{sup III} complexes can be efficiently sensitized by the ligand. - Graphical abstract: We present herein six lanthanide coordination polymers of a new semirigid exo-bidentate ligand which not only display diverse structures but also possess strong luminescence properties. - Highlights: • We present lanthanide coordination polymers of a new semirigid exo-bidentate ligand. • The lanthanide coordination polymers exhibit diverse structures. • The luminescent properties of Tb{sup III}, Eu{sup III} and Dy{sup III} complexes are discussed in detail.« less
  • Heterometallic carboxyphosphonates UO₂ 2+/Ln 3+ have been prepared from the hydrothermal reaction of uranyl nitrate, lanthanide nitrate (Ln = Sm, Tb, Er, Yb), and phosphonoacetic acid (H₃PPA). Compound 1, (UO₂)₂(PPA)(HPPA)₂Sm(H₂O)·2H₂O (1) adopts a two-dimensional structure in which the UO₂ 2+ metal ions bind exclusively to the phosphonate moiety, whereas the Ln 3+ ions are coordinated by both phosphonate and carboxylate functionalities. Luminescence studies of 1 show very bright visible and near-IR samarium(III)-centered emission upon direct excitation of the uranyl moiety. The Sm 3+ emissive state exhibits a double-exponential decay with lifetimes of 67.2 ± 6.5 and 9.0 ± 1.3 μsmore » as measured at 594 nm, after excitation at both 365 and 420 nm. No emission is observed in the region typical of the uranyl cation, indicating that all energy is either transferred to the Sm 3+ center or lost to nonradiative processes. Herein we report the synthesis, crystal structure, and luminescent behavior of 1, as well as those of the isostructural terbium, erbium, and ytterbium analogues.« less