Ligand-based reduction of CO(2) to CO mediated by an anionic niobium nitride complex

Journal of the American Chemical Society
Jared S Silvia, Christopher C Cummins

Abstract

The terminal nitride anion complex [Na][N[triple bond]Nb(N[(t)Bu]Ar)(3)] ([Na][1], Ar = 3,5-Me(2)C(6)H(3)) reacts quantitatively with CO(2) to give the carbamate complex [Na][O(2)CN[triple bond]Nb(N[(t)Bu]Ar)(3)] ([Na][O(2)C-1]). The structure of [Na][O(2)C-1] as the bis-12-crown-4 solvate, as determined by X-ray crystallography, displays a unique N-bound carbamate ligand without any metal-oxygen interactions. When treated with organic acid anhydrides or acid chlorides, complex [Na][O(2)C-1] reacts via salt elimination to give the five-coordinate complexes (RC(O)O)(OCN)Nb(N[(t)Bu]Ar)(3) (R-2, R = Me, (t)Bu, F(3)C). We show that complexes R-2 yield the starting complex [Na][1] with concomitant release of CO upon two-electron reduction. This series of reactions constitutes a closed cycle for the conversion of CO(2) to CO mediated by a terminal nitride anion complex.

References

Jul 19, 2002·Chemical Communications : Chem Comm·Justin K BraskChristopher C Cummins
Jun 24, 2004·Journal of the American Chemical Society·Christopher R CloughChristopher C Cummins
Aug 11, 2005·Journal of the American Chemical Society·Ingrid Castro-Rodriguez, Karsten Meyer
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Oct 26, 2006·Journal of the American Chemical Society·John J CurleyChristopher C Cummins
Nov 21, 2007·Angewandte Chemie·Brandi M Cossairt, Christopher C Cummins
Dec 23, 2008·Journal of the American Chemical Society·Jared S Silvia, Christopher C Cummins

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Citations

Aug 22, 2012·Inorganic Chemistry·Zachary ThammavongsyJohn D Gilbertson
Oct 15, 2011·Chemical Communications : Chem Comm·Zuofeng ChenThomas J Meyer
Jun 2, 2012·Proceedings of the National Academy of Sciences of the United States of America·Benedict M GardnerStephen T Liddle
Mar 10, 2016·Journal of the American Chemical Society·Tsun-Ren ChenKelvin H-C Chen
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