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Science 17 September 2004:
Vol. 305. no. 5691, pp. 1757 - 1759
DOI: 10.1126/science.1102602
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Reports

A Linear, O-Coordinated {eta}1-CO2 Bound to Uranium

Ingrid Castro-Rodriguez, Hidetaka Nakai, Lev N. Zakharov, Arnold L. Rheingold, Karsten Meyer*

The electron-rich, six-coordinate tris-aryloxide uranium(III) complex [((AdArO)3tacn)UIII] [where (AdArOH)3tacn = 1,4,7-tris(3-adamantyl-5-tert-butyl-2-hydroxybenzyl)1,4,7-triazacyclononane] reacts rapidly with CO2 to yield [((AdArO)3tacn)UIV(CO2)], a complex in which the CO2 ligand is linearly coordinated to the metal through its oxygen atom ({eta}1-OCO). The latter complex has been crystallographically and spectroscopically characterized. The inequivalent O–C–O bond lengths [1.122 angstroms (Å) for the O–C bond adjacent to uranium and 1.277 Å for the other], considered together with magnetization data and electronic and vibrational spectra, support the following bonding model: UIV=O=C{bullet}–O– {leftrightarrow} UIV–O{tbond}C–O–. In these charge-separated resonance structures, the uranium center is oxidized to uranium(IV) and the CO2 ligand reduced by one electron.

Department of Chemistry and Biochemistry, University of California, San Diego, 9500 Gilman Drive, MC 0358, La Jolla, CA 92093, USA.

* To whom correspondence should be addressed. E-mail: kmeyer{at}ucsd.edu

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