Carbon dioxide activation with sterically pressured mid- and high-valent uranium complexes

Journal of the American Chemical Society
Suzanne C BartKarsten Meyer

Abstract

Sterically pressured mid- to high-valent uranium complexes with an aryloxide substituted triazacyclononane ligand scaffold, [(((R)ArO)3tacn)(3-)], were studied for carbon dioxide activation and transformation chemistry. The high valent uranium(V) imido species [(((R)ArO)3tacn)U(NR)] (R = (t)Bu, R' = 2,4,6-trimethylphenyl (2-(t)Bu); R = Ad, R' = 2,4,6-trimethylphenyl (2-Ad); R = (t)Bu, R' = phenyl (3-(t)Bu)) were synthesized and spectroscopically characterized. X-ray crystallography of the tert-butyl mesityl imido derivative, 2-(t)Bu , reveals coordination of a bent imido fragment with a relatively long U-N bond distance of 2.05 A. The mesityl imido complexes reacted with carbon dioxide, readily extruding free isocyanate to produce uranium(V) terminal oxo species, [(((R)ArO)3tacn)U(O)] (R = (t)Bu (4-(t)Bu), Ad (4-Ad)), presumably through multiple bond metathesis via a uranium(V) carbimate intermediate. Using the smaller phenyl imido fragment in 3-(t) Bu slowed isocyanate loss, allowing the uranium(V) carbimate intermediate to undergo a second metathesis reaction, ultimately producing the diphenyl ureate derivative, [(((tBu)ArO)3tacn)U(NPh2)CO] (5-(t)Bu). Single crystal X-ray diffraction studies were carried out on both uranium(V...Continue Reading

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