volume 141 issue 2 pages 1016-1026

Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation.

Publication typeJournal Article
Publication date2018-12-11
scimago Q1
wos Q1
SJR5.554
CiteScore22.5
Impact factor15.6
ISSN00027863, 15205126
PubMed ID:  30532952
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
A series of uranyl compounds with the redox-active iminoquinone ligand have been synthesized, and their electronic structures elucidated using multinuclear NMR, EPR, electronic absorption spectroscopies, SQUID magnetometry, and X-ray crystallography. Characterization and analysis of the iminoquinone (iq0) complex, (dippiq)UO2(OTf)2THF (1-iq), the iminosemiquinone (isq1-) complex, (dippisq)2UO2THF (2-isq), and the amidophenolate (ap2-) complex, [(dippap)2UO2THF][K(18-crown-6)(THF)2]2(3-ap crown) show that reduction events are ligand-based, with the uranium center remaining in the hexavalent state. Reactivity of 2-isq with B-chlorocatecholborane or pivaloyl chloride leads to U-Ouranyl bond scission and reduction of U(VI) to U(IV) concomitant with ligand oxidation along with organic byproducts. 18O isotopic labeling experiments along with IR spectroscopy, mass spectrometry, and multinuclear NMR spectroscopy confirm that the organic byproducts contain oxygen atoms which originate from U-Ouranyl bond activation.
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Coughlin E. J. et al. Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation. // Journal of the American Chemical Society. 2018. Vol. 141. No. 2. pp. 1016-1026.
GOST all authors (up to 50) Copy
Coughlin E. J., Qiao Y., Lapsheva E., Zeller M., Schelter E. J., Bart S. C. Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation. // Journal of the American Chemical Society. 2018. Vol. 141. No. 2. pp. 1016-1026.
RIS |
Cite this
RIS Copy
TY - JOUR
DO - 10.1021/jacs.8b11302
UR - https://doi.org/10.1021/jacs.8b11302
TI - Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation.
T2 - Journal of the American Chemical Society
AU - Coughlin, Ezra J
AU - Qiao, Yusen
AU - Lapsheva, Ekaterina
AU - Zeller, Matthias
AU - Schelter, Eric J.
AU - Bart, Suzanne C.
PY - 2018
DA - 2018/12/11
PB - American Chemical Society (ACS)
SP - 1016-1026
IS - 2
VL - 141
PMID - 30532952
SN - 0002-7863
SN - 1520-5126
ER -
BibTex |
Cite this
BibTex (up to 50 authors) Copy
@article{2018_Coughlin,
author = {Ezra J Coughlin and Yusen Qiao and Ekaterina Lapsheva and Matthias Zeller and Eric J. Schelter and Suzanne C. Bart},
title = {Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation.},
journal = {Journal of the American Chemical Society},
year = {2018},
volume = {141},
publisher = {American Chemical Society (ACS)},
month = {dec},
url = {https://doi.org/10.1021/jacs.8b11302},
number = {2},
pages = {1016--1026},
doi = {10.1021/jacs.8b11302}
}
MLA
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MLA Copy
Coughlin, Ezra J., et al. “Uranyl Functionalization Mediated by Redox-Active Ligands: Generation of O-C Bonds via Acylation..” Journal of the American Chemical Society, vol. 141, no. 2, Dec. 2018, pp. 1016-1026. https://doi.org/10.1021/jacs.8b11302.