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Structure and spectroscopy of uranyl and thorium complexes with substituted phosphine oxide ligands

Breshears, Andrew T. and Barnes, Charles L. and Wagle, Durgesh V. and Baker, Gary A. and Takase, Michael K. and Walensky, Justin R. (2015) Structure and spectroscopy of uranyl and thorium complexes with substituted phosphine oxide ligands. Radiochimica Acta, 103 (1). pp. 49-56. ISSN 0033-8230. https://resolver.caltech.edu/CaltechAUTHORS:20150220-141447707

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Abstract

Phosphine oxide ligands are important in the chemistry of the nuclear fuel cycle. We have synthesized and characterized a series of phosphine oxide ligands with polycyclic aromatic hydrocarbon (PAH) groups to enhance the spectroscopic features of uranyl, UO_2^(2+), and to make detection more efficient. Complexation of OPPh_2R, R = C_(10)H_7 (naphthyl); C_(14)H_9 (phenanthrenyl); C_(14)H_9 (anthracenyl); and C_(16)H_9 (pyrenyl), to UO_2(NO_3)_2 afforded the eight-coordinate complexes, UO_2(NO_3)_2(OPPh_2R)_2. An eleven-coordinate complex, Th(NO_3)_4[OPPh_2(C_(14)H_9)]_3, C_(14)H_9 = phenanthrenyl, was structurally characterized, and was found to be the first thorium compound isolated with three phosphine oxide ligands bound. The phosphine oxide ligands were not fluorescent but the anthracenyl-substituted ligand showed broad, red-shifted emission at approximately 50 nm relative to typical anthracene, making this ligand set a possibility for use in detection. The synthesis and spectroscopy of the uranyl and thorium complexes are presented.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1515/ract-2014-2295DOIArticle
http://www.degruyter.com/view/j/ract.2015.103.issue-1/ract-2014-2295/ract-2014-2295.xmlPublisherArticle
ORCID:
AuthorORCID
Takase, Michael K.0000-0001-8365-3645
Additional Information:© 2014 by Walter de Gruyter GmbH. Received May 27, 2014; accepted September 11, 2014. This material is based upon work supported by the U.S. Department of Homeland Security under Grant Award Number, 2012-DN-130-NF0001-02. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security. We also acknowledge the Nuclear Regulatory Commission (NRC) Faculty Development Award for financial support.
Funders:
Funding AgencyGrant Number
Department of Homeland Security2012-DN-130-NF0001-02
Nuclear Regulatory Commission (NRC)UNSPECIFIED
Subject Keywords:Uranyl; Thorium; Phosphine Oxide; X-ray crystallography; Fluorescence
Issue or Number:1
Record Number:CaltechAUTHORS:20150220-141447707
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150220-141447707
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:55069
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:23 Feb 2015 20:02
Last Modified:09 Mar 2020 13:19

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