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Title: Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me 4N] 2[(AnO 2) 2(OH) 2(NO 3) 4]

Abstract

The synthesis of a series of molecular actinyl(VI), namely, uranium(VI), neptunium(VI), and plutonium(VI), hydroxo-bridged dimers is reported here. These complexes were isolated from an aqueous nitrate solution by titration with tetramethylammonium hydroxide. The solid-state structures were determined using single-crystal X-ray diffraction, revealing molecular complexes with the formula [Me 4N] 2[(AnO 2) 22-OH) 2(NO 3) 4], where An = U VI, Np VI, and Pu VI. Spectroscopic data—UV–vis–near-IR absorption, IR, and Raman—were collected on the solutions and solid-state complexes where available and compared to those of the aqueous solutions from which the crystals formed. These data provide structural evidence for higher-order polynuclear complexes of actinyl(VI) complexes upon a pH increase in the aqueous solution, confirming earlier thermodynamic models.

Authors:
 [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1509993
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 58; Journal Issue: 5; 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

Citation Formats

Autillo, Matthieu, and Wilson, Richard E. Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me4N]2[(AnO2)2(OH)2(NO3)4]. United States: N. p., 2019. Web. doi:10.1021/acs.inorgchem.8b03304.
Autillo, Matthieu, & Wilson, Richard E. Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me4N]2[(AnO2)2(OH)2(NO3)4]. United States. doi:10.1021/acs.inorgchem.8b03304.
Autillo, Matthieu, and Wilson, Richard E. Tue . "Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me4N]2[(AnO2)2(OH)2(NO3)4]". United States. doi:10.1021/acs.inorgchem.8b03304.
@article{osti_1509993,
title = {Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me4N]2[(AnO2)2(OH)2(NO3)4]},
author = {Autillo, Matthieu and Wilson, Richard E.},
abstractNote = {The synthesis of a series of molecular actinyl(VI), namely, uranium(VI), neptunium(VI), and plutonium(VI), hydroxo-bridged dimers is reported here. These complexes were isolated from an aqueous nitrate solution by titration with tetramethylammonium hydroxide. The solid-state structures were determined using single-crystal X-ray diffraction, revealing molecular complexes with the formula [Me4N]2[(AnO2)2(μ2-OH)2(NO3)4], where An = UVI, NpVI, and PuVI. Spectroscopic data—UV–vis–near-IR absorption, IR, and Raman—were collected on the solutions and solid-state complexes where available and compared to those of the aqueous solutions from which the crystals formed. These data provide structural evidence for higher-order polynuclear complexes of actinyl(VI) complexes upon a pH increase in the aqueous solution, confirming earlier thermodynamic models.},
doi = {10.1021/acs.inorgchem.8b03304},
journal = {Inorganic Chemistry},
number = 5,
volume = 58,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
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This content will become publicly available on February 12, 2020
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