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

Mei, Lei; Wang, Cong-zhi; Zhu, Liu-zheng; Gao, Zeng-qiang; Chai, Zhi-fang; Gibson, John K.; Shi, Wei-qun

doi:10.1021/acs.inorgchem.7b00312

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

Journal Article · Fri Jun 23 00:00:00 EDT 2017 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.7b00312 · OSTI ID:1436634

^[1]; Wang, Cong-zhi ^[1]; Zhu, Liu-zheng ^[1]; Gao, Zeng-qiang ^[2]; Chai, Zhi-fang ^[3];

^[4];

^[1]

Chinese Academy of Sciences (CAS), Beijing (China). Lab. of Nuclear Energy Chemistry. Inst. of High Energy Physics
Chinese Academy of Sciences (CAS), Beijing (China). Beijing Synchrotron Radiation Facility. Inst. of High Energy Physics
Chinese Academy of Sciences (CAS), Beijing (China). Lab. of Nuclear Energy Chemistry. Inst. of High Energy Physics; Soochow Univ., Suzhou (China). School of Radiological and Interdisciplinary Sciences. Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division

In this paper, the reaction of uranyl nitrate with terephthalic acid (H₂TP) 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. [UO₂(TP)_1.5](H₂BPP)_0.5·2H₂O (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, [(UO₂)₂(μ-OH)₂(TP)₂]₂(H₂BPP)₂·4.5H₂O (2). Another new polycatenated framework with a monomeric uranyl unit, [(UO₂)₂(TP)₃](H₂BPP) (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, [UO₂(TP)_1.5](H₂BPP)_0.5 (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 H₂TP linker. Finally, 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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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NSFC); Ministry of Industry and Information Technology of China

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1436634

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 14 Vol. 56; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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CCDC 1499906: Experimental Crystal Structure Determination: PECCOS : catena-[4,4'-(propane-1,3-diyl)di(pyridin-1-ium) tris(μ-benzene-1,4-dicarboxylato)-tetraoxo-di-uranium tetrahydrate] Mei, Lei; Wang, Cong-Zhi; Zhu, Liu-Zheng https://doi.org/10.5517/ccdc.csd.cc1mbs2t The current record is supplemented by this dataset	dataset	May 2017
CCDC 1499907: Experimental Crystal Structure Determination: PECCUY : catena-[4,4'-(propane-1,3-diyl)di(pyridin-1-ium) bis(μ-benzene-1,4-dicarboxylato)-bis(μ-hydroxo)-tetraoxo-di-uranium hydrate] Mei, Lei; Wang, Cong-Zhi; Zhu, Liu-Zheng https://doi.org/10.5517/ccdc.csd.cc1mbs3v The current record is supplemented by this dataset	dataset	May 2017
CCDC 1499908: Experimental Crystal Structure Determination: PECDAF : catena-[4,4'-(propane-1,3-diyl)di(pyridin-1-ium) tris(μ-benzene-1,4-dicarboxylato)-tetraoxo-di-uranium] Space Group: P 4 21 c (114), Cell: a 23.5464(3)Å b 23.5464(3)Å c 20.1023(3)Å, α 90° β 90° γ 90° Mei, Lei; Wang, Cong-Zhi; Zhu, Liu-Zheng https://doi.org/10.5517/ccdc.csd.cc1mbs4w The current record is supplemented by this dataset	dataset	May 2017
CCDC 1499909: Experimental Crystal Structure Determination: PECDEJ : catena-[4,4'-bipyridin-1-ium tris(μ-benzene-1,4-dicarboxylato)-tetraoxo-di-uranium] Mei, Lei; Wang, Cong-Zhi; Zhu, Liu-Zheng https://doi.org/10.5517/ccdc.csd.cc1mbs5x The current record is supplemented by this dataset	dataset	May 2017