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Title: Electronic structure and characterization of a uranyl di-15-crown-5 complex with an unprecedented sandwich structure

Abstract

Understanding of the nature and extent of chemical bonding in uranyl coordination complexes is crucial for the design of new ligands for nuclear waste separation, uranium extraction from seawater, and other applications. We report in this paper the synthesis, infrared spectroscopic characterization, and quantum chemical studies of a molecular uranyl–di-15-crown-5 complex. The structure and bonding of this unique complex featuring a distinctive 6-fold coplanar coordination staggered sandwich structure and an unusual non-perpendicular orientation of the uranyl moiety are evaluated using density functional theory and chemical bonding analyses. Finally, the results provide fundamental understanding of the coordination interaction of uranyl with oxygen-donor ligands.

Authors:
 [1];  [2];  [1];  [3];  [4];  [4];  [4];  [5]; ORCiD logo [1]
  1. Tsinghua Univ., Beijing (China). Dept. of Chemistry. Key Lab. of Organic Optoelectronics & Molecular Engineering of Ministry of Education
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  3. Duquesne Univ., Pittsburgh, PA (United States). Dept. of Chemistry and Biochemistry
  4. Radboud Univ., Nijmegen (Netherlands). Inst. for Molecules and Materials. FELIX Lab.
  5. Radboud Univ., Nijmegen (Netherlands). Inst. for Molecules and Materials. FELIX Lab.; Univ. of Amsterdam (Netherlands). Van't Hoff Inst. for Molecular Sciences
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tsinghua Univ., Beijing (China); Radboud Univ., Nijmegen (Netherlands)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC); Netherlands Organisation for Scientific Research (NWO)
OSTI Identifier:
1461101
Grant/Contract Number:  
AC02-05CH11231; 21433005; 91426302; 21590792; 724.011.002
Resource Type:
Accepted Manuscript
Journal Name:
ChemComm
Additional Journal Information:
Journal Volume: 52; Journal Issue: 86; Journal ID: ISSN 1359-7345
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hu, Shu-Xian, Gibson, John K., Li, Wan-Lu, Van Stipdonk, Michael J., Martens, Jonathan, Berden, Giel, Redlich, Britta, Oomens, Jos, and Li, Jun. Electronic structure and characterization of a uranyl di-15-crown-5 complex with an unprecedented sandwich structure. United States: N. p., 2016. Web. doi:10.1039/c6cc07205d.
Hu, Shu-Xian, Gibson, John K., Li, Wan-Lu, Van Stipdonk, Michael J., Martens, Jonathan, Berden, Giel, Redlich, Britta, Oomens, Jos, & Li, Jun. Electronic structure and characterization of a uranyl di-15-crown-5 complex with an unprecedented sandwich structure. United States. doi:10.1039/c6cc07205d.
Hu, Shu-Xian, Gibson, John K., Li, Wan-Lu, Van Stipdonk, Michael J., Martens, Jonathan, Berden, Giel, Redlich, Britta, Oomens, Jos, and Li, Jun. Wed . "Electronic structure and characterization of a uranyl di-15-crown-5 complex with an unprecedented sandwich structure". United States. doi:10.1039/c6cc07205d. https://www.osti.gov/servlets/purl/1461101.
@article{osti_1461101,
title = {Electronic structure and characterization of a uranyl di-15-crown-5 complex with an unprecedented sandwich structure},
author = {Hu, Shu-Xian and Gibson, John K. and Li, Wan-Lu and Van Stipdonk, Michael J. and Martens, Jonathan and Berden, Giel and Redlich, Britta and Oomens, Jos and Li, Jun},
abstractNote = {Understanding of the nature and extent of chemical bonding in uranyl coordination complexes is crucial for the design of new ligands for nuclear waste separation, uranium extraction from seawater, and other applications. We report in this paper the synthesis, infrared spectroscopic characterization, and quantum chemical studies of a molecular uranyl–di-15-crown-5 complex. The structure and bonding of this unique complex featuring a distinctive 6-fold coplanar coordination staggered sandwich structure and an unusual non-perpendicular orientation of the uranyl moiety are evaluated using density functional theory and chemical bonding analyses. Finally, the results provide fundamental understanding of the coordination interaction of uranyl with oxygen-donor ligands.},
doi = {10.1039/c6cc07205d},
journal = {ChemComm},
number = 86,
volume = 52,
place = {United States},
year = {2016},
month = {10}
}

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Works referenced in this record:

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  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
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Density‐functional thermochemistry. III. The role of exact exchange
journal, April 1993

  • Becke, Axel D.
  • The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652
  • DOI: 10.1063/1.464913