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Title: Homoleptic U(III) and U(IV) amidate complexes

Abstract

The syntheses of the first homoleptic U(III) and U(IV) amidate complexes are described here. These can be interconverted by chemical reduction/oxidation, showing an unusual change in coordination number from four in the U(III) complex to eight in the U(IV) complex in the solid state structures.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  2. 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); Univ. of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20); National Inst. of Health (NIH) (United States)
OSTI Identifier:
1505517
Grant/Contract Number:  
AC02-05CH11231; NA0003180; NA0000979; S10-RR027172
Resource Type:
Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 47; Journal Issue: 6; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Straub, M. D., Hohloch, S., Minasian, S. G., and Arnold, J. Homoleptic U(III) and U(IV) amidate complexes. United States: N. p., 2018. Web. doi:10.1039/c7dt04813k.
Straub, M. D., Hohloch, S., Minasian, S. G., & Arnold, J. Homoleptic U(III) and U(IV) amidate complexes. United States. doi:10.1039/c7dt04813k.
Straub, M. D., Hohloch, S., Minasian, S. G., and Arnold, J. Thu . "Homoleptic U(III) and U(IV) amidate complexes". United States. doi:10.1039/c7dt04813k. https://www.osti.gov/servlets/purl/1505517.
@article{osti_1505517,
title = {Homoleptic U(III) and U(IV) amidate complexes},
author = {Straub, M. D. and Hohloch, S. and Minasian, S. G. and Arnold, J.},
abstractNote = {The syntheses of the first homoleptic U(III) and U(IV) amidate complexes are described here. These can be interconverted by chemical reduction/oxidation, showing an unusual change in coordination number from four in the U(III) complex to eight in the U(IV) complex in the solid state structures.},
doi = {10.1039/c7dt04813k},
journal = {Dalton Transactions},
number = 6,
volume = 47,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 1 work
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Figures / Tables:

Figure 1 Figure 1: Binding modes of amidates to metal centers.

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    • Garner, Mary E.; Hohloch, Stephan; Maron, Laurent
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    Tantalum-Amidate Complexes for the Hydroaminoalkylation of Secondary Amines: Enhanced Substrate Scope and Enantioselective Chiral Amine Synthesis
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    Isolation of a Star-Shaped Uranium(V/VI) Cluster from the Anaerobic Photochemical Reduction of Uranyl(VI)
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    • DOI: 10.1002/chem.201200513

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    • DOI: 10.1002/zaac.200400024

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    • DOI: 10.1007/s12274-013-0379-6

    The crystal chemistry of uranium carboxylates
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    • DOI: 10.1016/j.ccr.2013.08.038

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    N , O -Chelating Four-Membered Metallacyclic Titanium(IV) Complexes for Atom-Economic Catalytic Reactions
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    • Gendron, Frédéric; Autschbach, Jochen
    • Journal of Chemical Theory and Computation, Vol. 12, Issue 11
    • DOI: 10.1021/acs.jctc.6b00462

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    Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework
    journal, April 2016


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    • ACS Applied Materials & Interfaces, Vol. 6, Issue 1
    • DOI: 10.1021/am404520b

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    • DOI: 10.1021/cr300198m

    Conjugates of Magnetic Nanoparticle—Actinide Specific Chelator for Radioactive Waste Separation
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    • Kaur, Maninder; Zhang, Huijin; Martin, Leigh
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    • DOI: 10.1021/es402205q

    Remediation of Soils and Wastes Contaminated with Uranium and Toxic Metals
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    • Francis, A. J.; Dodge, C. J.
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    • DOI: 10.1021/es9803310

    Synthesis and Structure of a Linked-Bis(amidate) Ligand and Some Complexes with Titanium
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    • Inorganic Chemistry, Vol. 40, Issue 23
    • DOI: 10.1021/ic010533o

    Environmental Speciation of Actinides
    journal, June 2012

    • Maher, Kate; Bargar, John R.; Brown, Gordon E.
    • Inorganic Chemistry, Vol. 52, Issue 7
    • DOI: 10.1021/ic301686d

    Synthesis and crystal structure of tris(cyclopentadienyl)pyrazolatouranium. A new mode of pyrazolate bonding
    journal, May 1981

    • Eigenbrot, Charles W.; Raymond, Kenneth N.
    • Inorganic Chemistry, Vol. 20, Issue 5
    • DOI: 10.1021/ic50219a043

    Reaction Chemistry of the U 3+ Metallocene Amidinate (C 5 Me 5 ) 2 [ i PrNC(Me)N i Pr]U Including the Isolation of a Uranium Complex of a Monodentate Acetate
    journal, February 2010

    • Evans, William J.; Walensky, Justin R.; Ziller, Joseph W.
    • Inorganic Chemistry, Vol. 49, Issue 4
    • DOI: 10.1021/ic902141f

    Functionalization of Carbon Dioxide and Carbon Disulfide Using a Stable Uranium(III) Alkyl Complex
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    • Matson, Ellen M.; Forrest, William P.; Fanwick, Phillip E.
    • Journal of the American Chemical Society, Vol. 133, Issue 13
    • DOI: 10.1021/ja110158s

    High-Valent Uranium Alkyls: Evidence for the Formation of U VI (CH 2 SiMe 3 ) 6
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    • DOI: 10.1021/ja204151v

    Identification of the +2 Oxidation State for Uranium in a Crystalline Molecular Complex, [K(2.2.2-Cryptand)][(C 5 H 4 SiMe 3 ) 3 U]
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    • DOI: 10.1021/ja406791t

    Uranium−Nitrogen Multiple Bonding: The Case of a Four-Coordinate Uranium(VI) Nitridoborate Complex
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    • Fox, Alexander R.; Cummins, Christopher C.
    • Journal of the American Chemical Society, Vol. 131, Issue 16
    • DOI: 10.1021/ja8095812

    Metal–Metal Bonding in Uranium–Group 10 Complexes
    journal, March 2016

    • Hlina, Johann A.; Pankhurst, James R.; Kaltsoyannis, Nikolas
    • Journal of the American Chemical Society, Vol. 138, Issue 10
    • DOI: 10.1021/jacs.5b10698

    Examining the Effects of Ligand Variation on the Electronic Structure of Uranium Bis(imido) Species
    journal, October 2016

    • Kiernicki, John J.; Ferrier, Maryline G.; Lezama Pacheco, Juan S.
    • Journal of the American Chemical Society, Vol. 138, Issue 42
    • DOI: 10.1021/jacs.6b06989

    A Homoleptic Uranium(III) Tris(aryl) Complex
    journal, December 2016

    • Boreen, Michael A.; Parker, Bernard F.; Lohrey, Trevor D.
    • Journal of the American Chemical Society, Vol. 138, Issue 49
    • DOI: 10.1021/jacs.6b11182

    A Thorium Chalcogenolate Series Generated by Atom Insertion into Thorium–Carbon Bonds
    journal, April 2017

    • Settineri, Nicholas S.; Garner, Mary E.; Arnold, John
    • Journal of the American Chemical Society, Vol. 139, Issue 17
    • DOI: 10.1021/jacs.7b02356

    Crystal Packing Forces Dictate η 1 - versus η 2 -Coordination of Benzyl Groups in [Guanidinate]Zr(CH 2 Ph) 3
    journal, July 2000

    • Giesbrecht, Garth R.; Whitener, Glenn D.; Arnold, John
    • Organometallics, Vol. 19, Issue 14
    • DOI: 10.1021/om000123s

    Solvent-Free Organometallic Reactivity: Synthesis of Hydride and Carboxylate Complexes of Uranium and Yttrium from Gas/Solid Reactions
    journal, December 2013

    • Webster, Christopher L.; Ziller, Joseph W.; Evans, William J.
    • Organometallics, Vol. 33, Issue 1
    • DOI: 10.1021/om401122d

    Actinide Amidinate Complexes with a Dimethylamine Side Arm: Synthesis, Structural Characterization, and Reactivity
    journal, January 2015

    • Karmel, Isabell S. R.; Fridman, Natalia; Eisen, Moris S.
    • Organometallics, Vol. 34, Issue 3
    • DOI: 10.1021/om501179e

    Insertion of Carbodiimides and Organic Azides into Actinide−Carbon Bonds
    journal, June 2009

    • Evans, William J.; Walensky, Justin R.; Ziller, Joseph W.
    • Organometallics, Vol. 28, Issue 12
    • DOI: 10.1021/om900135e

    Insertion Reactivity of CO 2 , PhNCO, Me 3 CC≡N, and Me 3 CN≡C with the Uranium−Alkynyl Bonds in (C 5 Me 5 ) 2 U(C≡CPh) 2
    journal, February 2010

    • Evans, William J.; Walensky, Justin R.; Ziller, Joseph W.
    • Organometallics, Vol. 29, Issue 4
    • DOI: 10.1021/om901006t

    Uranium-mediated electrocatalytic dihydrogen production from water
    journal, January 2016

    • Halter, Dominik P.; Heinemann, Frank W.; Bachmann, Julien
    • Nature, Vol. 530, Issue 7590
    • DOI: 10.1038/nature16530

    Nitrogen reduction and functionalization by a multimetallic uranium nitride complex
    journal, July 2017

    • Falcone, Marta; Chatelain, Lucile; Scopelliti, Rosario
    • Nature, Vol. 547, Issue 7663
    • DOI: 10.1038/nature23279

    Uranium azide photolysis results in C–H bond activation and provides evidence for a terminal uranium nitride
    journal, July 2010

    • Thomson, Robert K.; Cantat, Thibault; Scott, Brian L.
    • Nature Chemistry, Vol. 2, Issue 9
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    Pentavalent uranium chemistry—synthetic pursuit of a rare oxidation state
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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.