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Title: Structural and spectroscopic studies of a rare non-oxido V(v) complex crystallized from aqueous solution

Abstract

A non-oxido V(v) complex with glutaroimide-dioxime (H3L), a ligand for recovering uranium from seawater, was synthesized from aqueous solution as Na[V(L)2]·2H2O, and the structure determined by X-ray diffraction. It is the first non-oxido V(v) complex that has been directly synthesized in and crystallized from aqueous solution. The distorted octahedral structure contains two fully deprotonated ligands (L3-) coordinating to V5+, each in a tridentate mode via the imide N (RV-N = 1.96 Å) and oxime O atoms (RV-O = 1.87-1.90 Å). Using 17O-labelled vanadate as the starting material, concurrent 17O/ 51V/ 1H/ 13C NMR, in conjunction with ESI-MS, unprecedentedly demonstrated the stepwise displacement of the oxido V=O bonds by glutaroimide-dioxime and verified the existence of the "bare" V5+ /glutaroimide-dioxime complex, [V(L)2] - , in aqueous solution. In addition, the crystal structure of an intermediate 1 : 1 V(v)/glutaroimide-dioxime complex, [VO2(HL)] - , in which the oxido bonds of vanadate are only partially displaced, corroborates the observations by NMR and ESI-MS. Results from this work provide important insights into the strong sorption of vanadium on poly(amidoxime) sorbents in the recovery of uranium from seawater. Also, because vanadium plays important roles in biological systems, the syntheses of the oxido and non-oxido V5+ complexesmore » and the unprecedented demonstration of the displacement of the oxido V=O bonds help with the on-going efforts to develop new vanadium compounds that could be of importance in biological applications.« less

Authors:
 [1];  [2];  [3];  [1];  [1];  [1];  [4];  [5];  [4];  [1];  [2];  [1]
  1. 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; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). National Security Directorate
  5. Fundamental and Computational Sciences Directorate; Pacific Northwest National Laboratory; Richland, USA
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1377416
Alternate Identifier(s):
OSTI ID: 1337242
Report Number(s):
PNNL-SA-112588
Journal ID: ISSN 2041-6520; CSHCBM; ark:/13030/qt2p03j1ms
Grant/Contract Number:  
AC02-05CH11231; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 7; Journal Issue: 4; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; vanadium; uranium; seawater; amidoxime; XRD

Citation Formats

Leggett, C. J., Parker, B. F., Teat, S. J., Zhang, Z., Dau, P. D., Lukens, W. W., Peterson, S. M., Cardenas, A. J. P., Warner, M. G., Gibson, J. K., Arnold, J., and Rao, L. Structural and spectroscopic studies of a rare non-oxido V(v) complex crystallized from aqueous solution. United States: N. p., 2016. Web. doi:10.1039/c5sc03958d.
Leggett, C. J., Parker, B. F., Teat, S. J., Zhang, Z., Dau, P. D., Lukens, W. W., Peterson, S. M., Cardenas, A. J. P., Warner, M. G., Gibson, J. K., Arnold, J., & Rao, L. Structural and spectroscopic studies of a rare non-oxido V(v) complex crystallized from aqueous solution. United States. doi:10.1039/c5sc03958d.
Leggett, C. J., Parker, B. F., Teat, S. J., Zhang, Z., Dau, P. D., Lukens, W. W., Peterson, S. M., Cardenas, A. J. P., Warner, M. G., Gibson, J. K., Arnold, J., and Rao, L. Thu . "Structural and spectroscopic studies of a rare non-oxido V(v) complex crystallized from aqueous solution". United States. doi:10.1039/c5sc03958d. https://www.osti.gov/servlets/purl/1377416.
@article{osti_1377416,
title = {Structural and spectroscopic studies of a rare non-oxido V(v) complex crystallized from aqueous solution},
author = {Leggett, C. J. and Parker, B. F. and Teat, S. J. and Zhang, Z. and Dau, P. D. and Lukens, W. W. and Peterson, S. M. and Cardenas, A. J. P. and Warner, M. G. and Gibson, J. K. and Arnold, J. and Rao, L.},
abstractNote = {A non-oxido V(v) complex with glutaroimide-dioxime (H3L), a ligand for recovering uranium from seawater, was synthesized from aqueous solution as Na[V(L)2]·2H2O, and the structure determined by X-ray diffraction. It is the first non-oxido V(v) complex that has been directly synthesized in and crystallized from aqueous solution. The distorted octahedral structure contains two fully deprotonated ligands (L3-) coordinating to V5+, each in a tridentate mode via the imide N (RV-N = 1.96 Å) and oxime O atoms (RV-O = 1.87-1.90 Å). Using 17O-labelled vanadate as the starting material, concurrent 17O/ 51V/ 1H/ 13C NMR, in conjunction with ESI-MS, unprecedentedly demonstrated the stepwise displacement of the oxido V=O bonds by glutaroimide-dioxime and verified the existence of the "bare" V5+ /glutaroimide-dioxime complex, [V(L)2] - , in aqueous solution. In addition, the crystal structure of an intermediate 1 : 1 V(v)/glutaroimide-dioxime complex, [VO2(HL)] - , in which the oxido bonds of vanadate are only partially displaced, corroborates the observations by NMR and ESI-MS. Results from this work provide important insights into the strong sorption of vanadium on poly(amidoxime) sorbents in the recovery of uranium from seawater. Also, because vanadium plays important roles in biological systems, the syntheses of the oxido and non-oxido V5+ complexes and the unprecedented demonstration of the displacement of the oxido V=O bonds help with the on-going efforts to develop new vanadium compounds that could be of importance in biological applications.},
doi = {10.1039/c5sc03958d},
journal = {Chemical Science},
number = 4,
volume = 7,
place = {United States},
year = {2016},
month = {1}
}

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Works referenced in this record:

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    Works referencing / citing this record:

    An anionic manganese( ii ) metal–organic framework for uranyl adsorption
    journal, January 2019

    • Zhang, Tao; Ling, Bo-Kai; Hu, Yue-Qiao
    • CrystEngComm, Vol. 21, Issue 26
    • DOI: 10.1039/c9ce00603f

    The chemical nature of amavadin
    journal, January 1993

    • Armstrong, Elaine M.; Beddoes, Roy L.; Calviou, Louise J.
    • Journal of the American Chemical Society, Vol. 115, Issue 2
    • DOI: 10.1021/ja00055a073

    Siderophore-inspired chelator hijacks uranium from aqueous medium
    journal, February 2019

    • Ivanov, Alexander S.; Parker, Bernard F.; Zhang, Zhicheng
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-08758-1

    Structural and redox requirements for the action of anti-diabetic vanadium compounds
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    2,6-Diiminopiperidin-1-ol: an overlooked motif relevant to uranyl and transition metal binding on poly(amidoxime) adsorbents
    journal, January 2016

    • Kennedy, Zachary C.; Cardenas, Allan Jay P.; Corbey, Jordan F.
    • Chemical Communications, Vol. 52, Issue 57
    • DOI: 10.1039/c6cc02488b

    Redox Chemistry of Actinide Ions in Wells−Dawson Heteropolyoxoanion Complexes
    journal, August 2003

    • Chiang, Ming-Hsi; Soderholm, L.; Antonio, Mark R.
    • European Journal of Inorganic Chemistry, Vol. 2003, Issue 16
    • DOI: 10.1002/ejic.200300225

    Cost Estimation of Uranium Recovery from Seawater with System of Braid Type Adsorbent [モール状捕集システムによる海水ウラン捕集のコスト試算]
    journal, January 2006

    • Tamada, Masao; Seko, Noriaki; Kasai, Noboru
    • Transactions of the Atomic Energy Society of Japan, Vol. 5, Issue 4
    • DOI: 10.3327/taesj2002.5.358

    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

    Vanadium (IV) and vanadium (V) complexes of deferoxamine B in aqueous solution
    journal, October 1995


    Extraction of Uranium from Sea Water
    journal, September 1964

    • Davies, R. V.; Kennedy, J.; McILROY, R. W.
    • Nature, Vol. 203, Issue 4950
    • DOI: 10.1038/2031110a0

    Synthesis, structural and physicochemical characterization of a new type Ti 6 -oxo cluster protected by a cyclic imide dioxime ligand
    journal, January 2019

    • Passadis, Stamatis S.; Hadjithoma, Sofia; Kalampounias, Angelos G.
    • Dalton Transactions, Vol. 48, Issue 17
    • DOI: 10.1039/c9dt00658c

    Particulate and dissolved vanadium in the North Pacific Ocean
    journal, May 1984


    Complexation of glutarimidedioxime with Fe(iii), Cu(ii), Pb(ii), and Ni(ii), the competing ions for the sequestration of U(vi) from seawater
    journal, January 2013

    • Sun, Xiaoqi; Xu, Chao; Tian, Guoxin
    • Dalton Transactions, Vol. 42, Issue 40
    • DOI: 10.1039/c3dt51767e

    Vanadium(V) oxyanions. Interactions of vanadate with oxalate, lactate and glycerate
    journal, March 1987

    • Tracey, Alan S.; Gresser, Michael J.; Parkinson, Kevin M.
    • Inorganic Chemistry, Vol. 26, Issue 5
    • DOI: 10.1021/ic00252a002

    Interactions of vanadium( iv ) with amidoxime ligands: redox reactivity
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    • Parker, B. F.; Hohloch, S.; Pankhurst, J. R.
    • Dalton Transactions, Vol. 47, Issue 16
    • DOI: 10.1039/c7dt04069e

    Uptake of Uranium from Seawater by Amidoxime-Based Polymeric Adsorbent: Field Experiments, Modeling, and Updated Economic Assessment
    journal, March 2014

    • Kim, Jungseung; Tsouris, Costas; Oyola, Yatsandra
    • Industrial & Engineering Chemistry Research, Vol. 53, Issue 14
    • DOI: 10.1021/ie4039828

    Stereochemistry of dioxovanadium(V) complexes. III. Crystal and molecular structures of trisodium (ethylenediaminetraacetato)dioxovanadate(V) tetrahydrate
    journal, August 1971

    • Hoard, J. L.; Scheidt, W. Robert; Countryman, R.
    • Journal of the American Chemical Society, Vol. 93, Issue 16
    • DOI: 10.1021/ja00745a008

    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

    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

    Vanadium-51 NMR
    journal, January 1990


    Stereochemistry and total synthesis of amavadin, the naturally occurring vanadium compound of Amanita muscaria
    journal, May 1986

    • Kneifel, H.; Bayer, E.
    • Journal of the American Chemical Society, Vol. 108, Issue 11
    • DOI: 10.1021/ja00271a043

    The first enantioselective synthesis of the amavadin ligand and its complexation to vanadium
    journal, May 2005


    Complex Formation of Vanadium(IV) with 1,3,5-Triamino-1,3,5-trideoxy- cis -inositol and Related Ligands
    journal, May 2004

    • Morgenstern, Bernd; Steinhauser, Stefan; Hegetschweiler, Kaspar
    • Inorganic Chemistry, Vol. 43, Issue 10
    • DOI: 10.1021/ic0352046

    Recovery of Uranium from Seawater: A Review of Current Status and Future Research Needs
    journal, January 2013


    Amavadin, a vanadium natural complex: Its role and applications
    journal, August 2013

    • da Silva, José A. L.; Fraústo da Silva, João J. R.; Pombeiro, Armando J. L.
    • Coordination Chemistry Reviews, Vol. 257, Issue 15-16
    • DOI: 10.1016/j.ccr.2013.03.010

    Siderophore-inspired chelator hijacks uranium from aqueous medium
    journal, February 2019

    • Ivanov, Alexander S.; Parker, Bernard F.; Zhang, Zhicheng
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-08758-1

    2,6-Diiminopiperidin-1-ol: an overlooked motif relevant to uranyl and transition metal binding on poly(amidoxime) adsorbents
    journal, January 2016

    • Kennedy, Zachary C.; Cardenas, Allan Jay P.; Corbey, Jordan F.
    • Chemical Communications, Vol. 52, Issue 57
    • DOI: 10.1039/c6cc02488b

    Interactions of vanadium( iv ) with amidoxime ligands: redox reactivity
    journal, January 2018

    • Parker, B. F.; Hohloch, S.; Pankhurst, J. R.
    • Dalton Transactions, Vol. 47, Issue 16
    • DOI: 10.1039/c7dt04069e

    An anionic manganese( ii ) metal–organic framework for uranyl adsorption
    journal, January 2019

    • Zhang, Tao; Ling, Bo-Kai; Hu, Yue-Qiao
    • CrystEngComm, Vol. 21, Issue 26
    • DOI: 10.1039/c9ce00603f

    Synthesis, structural and physicochemical characterization of a new type Ti 6 -oxo cluster protected by a cyclic imide dioxime ligand
    journal, January 2019

    • Passadis, Stamatis S.; Hadjithoma, Sofia; Kalampounias, Angelos G.
    • Dalton Transactions, Vol. 48, Issue 17
    • DOI: 10.1039/c9dt00658c