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Title: A Uranyl Metal Organic Framework Arising from the Coordination of a Partially Hydrolyzed Tetrauranyl Node with the Tautomerically Diverse 1,4-(diamidoximyl)benzene Ligand

Abstract

We report a unique uranium-based metal organic framework afforded from the spontaneous reaction of 1,4-(diamidoximyl)benzene (1,4-(DAO)Bz) with uranyl chloride. The structure is the first reported example to show either hydrolysis alongside amidoxime coordination or the presence of multiple amidoxime protonation states in a single complex. The ability of the ligand to adopt three chemically distinct forms affords it enough flexibility to link the typically planar uranyl nodes in three orthogonal directions, giving rise to a cationic framework with large channels and suggesting applications for this system in crystal engineering.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Univ. of Alabama, Tuscaloosa, AL (United States)
  2. Univ. of Missouri, Columbia, MO (United States)
  3. Univ. of Alabama, Tuscaloosa, AL (United States); 525 Solutions, Inc., Tuscaloosa, AL (United States)
Publication Date:
Research Org.:
Univ. of Alabama, Tuscaloosa, AL (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
OSTI Identifier:
1558201
Alternate Identifier(s):
OSTI ID: 1592763; OSTI ID: 1592764
Report Number(s):
DOE-UA-08427
Journal ID: ISSN 1528-7483
Grant/Contract Number:  
NE0008427
Resource Type:
Accepted Manuscript
Journal Name:
Crystal Growth and Design
Additional Journal Information:
Journal Volume: 19; Journal Issue: 10; Related Information: CCDC No. 1862662 (crystal structure data); Journal ID: ISSN 1528-7483
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Metal Organic Framework; 1,4-(diamidoximyl)benzene; Metal Organic Framework, 1,4-(diamidoximyl)benzene

Citation Formats

Mishra, Manish Kumar, Patil, Yogesh, Kelley, Steven P., and Rogers, Robin D. A Uranyl Metal Organic Framework Arising from the Coordination of a Partially Hydrolyzed Tetrauranyl Node with the Tautomerically Diverse 1,4-(diamidoximyl)benzene Ligand. United States: N. p., 2019. Web. doi:10.1021/acs.cgd.9b00544.
Mishra, Manish Kumar, Patil, Yogesh, Kelley, Steven P., & Rogers, Robin D. A Uranyl Metal Organic Framework Arising from the Coordination of a Partially Hydrolyzed Tetrauranyl Node with the Tautomerically Diverse 1,4-(diamidoximyl)benzene Ligand. United States. https://doi.org/10.1021/acs.cgd.9b00544
Mishra, Manish Kumar, Patil, Yogesh, Kelley, Steven P., and Rogers, Robin D. Wed . "A Uranyl Metal Organic Framework Arising from the Coordination of a Partially Hydrolyzed Tetrauranyl Node with the Tautomerically Diverse 1,4-(diamidoximyl)benzene Ligand". United States. https://doi.org/10.1021/acs.cgd.9b00544. https://www.osti.gov/servlets/purl/1558201.
@article{osti_1558201,
title = {A Uranyl Metal Organic Framework Arising from the Coordination of a Partially Hydrolyzed Tetrauranyl Node with the Tautomerically Diverse 1,4-(diamidoximyl)benzene Ligand},
author = {Mishra, Manish Kumar and Patil, Yogesh and Kelley, Steven P. and Rogers, Robin D.},
abstractNote = {We report a unique uranium-based metal organic framework afforded from the spontaneous reaction of 1,4-(diamidoximyl)benzene (1,4-(DAO)Bz) with uranyl chloride. The structure is the first reported example to show either hydrolysis alongside amidoxime coordination or the presence of multiple amidoxime protonation states in a single complex. The ability of the ligand to adopt three chemically distinct forms affords it enough flexibility to link the typically planar uranyl nodes in three orthogonal directions, giving rise to a cationic framework with large channels and suggesting applications for this system in crystal engineering.},
doi = {10.1021/acs.cgd.9b00544},
journal = {Crystal Growth and Design},
number = 10,
volume = 19,
place = {United States},
year = {2019},
month = {8}
}

Works referenced in this record:

Chemical Forms of Uranium in Artificial Seawater
journal, February 1982


Development of Sorbers for the Recovery of Uranium from Seawater. 1. Assessment of Key Parameters and Screening Studies of Sorber Materials
journal, August 1982

  • Schenk, H. J.; Astheimer, L.; Witte, E. G.
  • Separation Science and Technology, Vol. 17, Issue 11
  • DOI: 10.1080/01496398208056103

Coordination chemistry and metal-involving reactions of amidoximes: Relevance to the chemistry of oximes and oxime ligands
journal, April 2016

  • Bolotin, Dmitrii S.; Bokach, Nadezhda A.; Kukushkin, Vadim Yu.
  • Coordination Chemistry Reviews, Vol. 313
  • DOI: 10.1016/j.ccr.2015.10.005

Materials for the Recovery of Uranium from Seawater
journal, June 2017


Cyclic Imide Dioximes: Formation and Hydrolytic Stability
journal, May 2012

  • Kang, Sung Ok; Vukovic, Sinisa; Custelcean, Radu
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 19
  • DOI: 10.1021/ie300492z

An overview and recent progress in the chemistry of uranium extraction from seawater
journal, January 2018

  • Parker, B. F.; Zhang, Z.; Rao, L.
  • Dalton Transactions, Vol. 47, Issue 3
  • DOI: 10.1039/C7DT04058J

Uranyl complexes of acetamidoxime and benzamidoxime. Preparation, characterization, and crystal structure
journal, June 1984


Highly selective extraction of the uranyl ion with hydrophobic amidoxime-functionalized ionic liquids via η2 coordination
journal, January 2012

  • Barber, Patrick S.; Kelley, Steven P.; Rogers, Robin D.
  • RSC Advances, Vol. 2, Issue 22
  • DOI: 10.1039/c2ra21344c

How Amidoximate Binds the Uranyl Cation
journal, February 2012

  • Vukovic, Sinisa; Watson, Lori A.; Kang, Sung Ok
  • Inorganic Chemistry, Vol. 51, Issue 6
  • DOI: 10.1021/ic300062s

Sequestering uranium from seawater: binding strength and modes of uranyl complexes with glutarimidedioxime
journal, January 2012

  • Tian, Guoxin; Teat, Simon J.; Zhang, Zhiyong
  • Dalton Transactions, Vol. 41, Issue 38
  • DOI: 10.1039/c2dt30978e

Structural clues to UO 2 2+ /VO 2 + competition in seawater extraction using amidoxime-based extractants
journal, January 2014

  • Kelley, Steven P.; Barber, Patrick S.; Mullins, Peter H. K.
  • Chem. Commun., Vol. 50, Issue 83
  • DOI: 10.1039/C4CC06370H

Hydrogen bond patterns in aromatic and aliphatic dioximes
journal, January 2003

  • Bruton, Eric A.; Brammer, Lee; Christopher Pigge, F.
  • New J. Chem., Vol. 27, Issue 7
  • DOI: 10.1039/B301045G

Species Distribution and Coordination of Uranyl Chloro Complexes in Acetonitrile
journal, March 2008

  • Hennig, Christoph; Servaes, Kelly; Nockemann, Peter
  • Inorganic Chemistry, Vol. 47, Issue 8
  • DOI: 10.1021/ic7014435

First Structurally Characterized Actinide Isocyanates
journal, November 2004

  • Crawford, Margaret-Jane; Mayer, Peter; Nöth, Heinrich
  • Inorganic Chemistry, Vol. 43, Issue 22
  • DOI: 10.1021/ic049078x

U6+ Minerals and Inorganic Compounds: Insights into an Expanded Structural Hierarchy of Crystal Structures
journal, December 2005


An uranyl citrate coordination polymer with a 3D open-framework involving uranyl cation-cation interactions
journal, January 2011

  • Lhoste, Jérôme; Henry, Natacha; Roussel, Pascal
  • Dalton Transactions, Vol. 40, Issue 11
  • DOI: 10.1039/c0dt01721c

Occurence of an Octanuclear Motif of Uranyl Isophthalate with Cation–Cation Interactions through Edge-Sharing Connection Mode
journal, July 2011

  • Mihalcea, Ionut; Henry, Natacha; Clavier, Nicolas
  • Inorganic Chemistry, Vol. 50, Issue 13
  • DOI: 10.1021/ic2005584

Mixed Formate-Dicarboxylate Coordination Polymers with Tetravalent Uranium: Occurrence of Tetranuclear {U 4 O 4 } and Hexanuclear {U 6 O 4 (OH) 4 } Motifs
journal, June 2013

  • Falaise, Clément; Volkringer, Christophe; Loiseau, Thierry
  • Crystal Growth & Design, Vol. 13, Issue 7
  • DOI: 10.1021/cg400643g

Novel Uranyl Coordination Polymers Based on Quinoline-Containing Dicarboxylate by Altering Auxiliary Ligands: From 1D Chain to 3D Framework
journal, July 2016

  • Hu, Kong-Qiu; Zhu, Liu-Zheng; Wang, Cong-Zhi
  • Crystal Growth & Design, Vol. 16, Issue 9
  • DOI: 10.1021/acs.cgd.6b00429

Three-Dimensional Hybrid Framework Containing U 2 O 13 Dimers Connected via Cation–Cation Interactions
journal, September 2011

  • Severance, Rachel C.; Smith, Mark D.; zur Loye, Hans-Conrad
  • Inorganic Chemistry, Vol. 50, Issue 17
  • DOI: 10.1021/ic200985m

An Anionic Uranium-Based Metal–Organic Framework with Ultralarge Nanocages for Selective Dye Adsorption
journal, January 2018