| SYNTHESIS |
N2 to amides in a single pot Key steps in the conversion of dinitrogen to ammonia can be carried out in a one-pot synthesis procedure, according to researchers at the University of Ottawa. Sandro Gambarotta, Ilia Korobkov, and coworkers report that a transient midvalent thorium complex generated via a reaction between zero- and tetravalent thorium complexes can be used to promote N2 bond cleavage and hydrogenation in a single-step reaction that transforms the gas into amides [Angew. Chem. Int. Ed., 42, 4958 (2003)]. Previous work in nitrogen-activation chemistry by other researchers has led to separate synthesis procedures for each of these steps. Although the mechanism has not yet been elucidated, the Ottawa group proposes that the reaction involves the midvalent complex and a zero-valent thorium species (shown), which they have isolated and analyzed with X-ray crystallography. The most likely route for the reaction, they say, is by way of cooperative attack on a single N2 unit by two or more metal centers, which cleaves the molecule, and hydrogenation of N via radical-based H abstraction from the solvent. |
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