Synthesis, characterization, and reactivity of a uranyl beta-diketiminate complex

Journal of the American Chemical Society
Trevor W Hayton, Guang Wu

Abstract

Addition of 1 equiv of Li(Ar2nacnac) (Ar2nacnac = (2,6-(i)Pr2C6H3)NC(Me)CHC(Me)N(2,6-(i)Pr2C6H3)) to an Et2O suspension of UO2Cl2(THF)3 generates the uranyl dimer [UO2(Ar2nacnac)Cl]2 (1) in good yield. A second species can be isolated in low yield from the reaction mixtures of 1, namely [Li(OEt2)2][UO2(Ar2nacnac)Cl2] (2). The structures of both 1 and 2 have been confirmed by X-ray crystallography. Complex 1 reacts with Ph3PO to generate UO2(Ar2nacnac)Cl(Ph3PO) (3). In addition, 1 reacts with AgOTf and either 1 equiv of DPPMO2 or 2 equiv of Ph2MePO to provide [UO2(Ar2nacnac)(DPPMO2)][OTf] (4) and [UO2(Ar2nacnac)(Ph2MePO)2][OTf] (5), respectively. Both 4 and 5 have been fully characterized, including analysis by X-ray crystallography and cyclic voltammetry. Reduction of 4 with Cp2Co provides UO2(Ar2nacnac)(CH{Ph2PO}2) (6), a uranyl(VI) complex that is generated by the formal loss of H* from the DPPMO2 ligand. Labeling studies have been performed in an attempt to elucidate the mechanism of hydrogen loss. In contrast, reduction of 5 with Cp2Co provides UO2(Ar2nacnac)(Ph2MePO)2 (7), a rare example of a uranyl(V) complex. As expected, the solid-state molecular structure of 7 reveals slightly longer U-O(oxo) bond lengths relative to 5...Continue Reading

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Citations

Nov 8, 2012·Chemical Reviews·Matthew B Jones, Andrew J Gaunt
Mar 26, 2009·Chemical Communications : Chem Comm·Pawel HoregladMarinella Mazzanti
Aug 8, 2009·Chemical Communications : Chem Comm·Christopher R Graves, Jaqueline L Kiplinger
Jul 10, 2009·Chemical Communications : Chem Comm·Jason B Love
Oct 20, 2010·Chemical Communications : Chem Comm·Victor MougelMarinella Mazzanti
Jan 18, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Lucile ChatelainMarinella Mazzanti
Dec 17, 2009·Journal of the American Chemical Society·Grégory NoctonMarinella Mazzanti
Nov 6, 2010·Chemistry : a European Journal·Victor MougelMarinella Mazzanti
May 8, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Roy CoppingMark J Sarsfield
Jan 28, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Trevor W Hayton
Oct 3, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Nicholas E TraviaJaqueline L Kiplinger
Jun 5, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Michael A BoreenJohn Arnold
Nov 15, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·Jie ZhangXigeng Zhou
Oct 16, 2018·Chemical Science·Radmila FaizovaMarinella Mazzanti
Mar 25, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·Ulrich SiemelingPetr Štěpnička
Dec 3, 2011·Chemical Communications : Chem Comm·Victor MougelMarinella Mazzanti
Sep 30, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Stephan HohlochJohn Arnold
May 3, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Neil C TomsonJames M Boncella
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Nov 17, 2012·Chemistry : a European Journal·Robert J Baker
Aug 25, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Florian DulongThibault Cantat
Jan 12, 2021·Angewandte Chemie·Radmila FaizovaMarinella Mazzanti
Dec 5, 2008·Inorganic Chemistry·Christopher R GravesJaqueline L Kiplinger
Dec 2, 2009·Inorganic Chemistry·Michael F SchettiniTrevor W Hayton
Dec 2, 2009·Inorganic Chemistry·Liam P SpencerJames M Boncella
Sep 17, 2009·Inorganic Chemistry·Koichiro TakaoChristoph Hennig
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Jun 8, 2012·Journal of the American Chemical Society·Robert E JilekJames M Boncella
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May 27, 2015·Inorganic Chemistry·Clément CampMarinella Mazzanti
May 16, 2017·Inorganic Chemistry·Elizabeth A PedrickTrevor W Hayton
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Oct 6, 2018·Journal of the American Chemical Society·Radmila FaizovaMarinella Mazzanti
Jan 25, 2020·Inorganic Chemistry·Judith RiedhammerDaniel J Mindiola

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