Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks
Abstract
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),more »
- Authors:
-
[1];
[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
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Ministry of Industry and Information Technology of China
- OSTI Identifier:
- 1436634
- Grant/Contract Number:
- AC02-05CH11231; 21671191; 21577144; 11405186; 91426302; 91326202; JCKY2016212A504
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 56; Journal Issue: 14; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Mei, Lei, Wang, Cong-zhi, Zhu, Liu-zheng, Gao, Zeng-qiang, Chai, Zhi-fang, Gibson, John K., and Shi, Wei-qun. Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks. United States: N. p., 2017.
Web. doi:10.1021/acs.inorgchem.7b00312.
Mei, Lei, Wang, Cong-zhi, Zhu, Liu-zheng, Gao, Zeng-qiang, Chai, Zhi-fang, Gibson, John K., & Shi, Wei-qun. Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks. United States. https://doi.org/10.1021/acs.inorgchem.7b00312
Mei, Lei, Wang, Cong-zhi, Zhu, Liu-zheng, Gao, Zeng-qiang, Chai, Zhi-fang, Gibson, John K., and Shi, Wei-qun. Fri .
"Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks". United States. https://doi.org/10.1021/acs.inorgchem.7b00312. https://www.osti.gov/servlets/purl/1436634.
@article{osti_1436634,
title = {Exploring New Assembly Modes of Uranyl Terephthalate: Templated Syntheses and Structural Regulation of a Series of Rare 2D → 3D Polycatenated Frameworks},
author = {Mei, Lei and Wang, Cong-zhi and Zhu, Liu-zheng and Gao, Zeng-qiang and Chai, Zhi-fang and Gibson, John K. and Shi, Wei-qun},
abstractNote = {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.},
doi = {10.1021/acs.inorgchem.7b00312},
journal = {Inorganic Chemistry},
number = 14,
volume = 56,
place = {United States},
year = {Fri Jun 23 00:00:00 EDT 2017},
month = {Fri Jun 23 00:00:00 EDT 2017}
}
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