Catalytic Reduction of Dinitrogen to Ammonia at a Single Molybdenum Center

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Science  04 Jul 2003:
Vol. 301, Issue 5629, pp. 76-78
DOI: 10.1126/science.1085326

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Dinitrogen (N2) was reduced to ammonia at room temperature and 1 atmosphere with molybdenum catalysts that contain tetradentate [HIPTN3N]3– triamidoamine ligands {such as [HIPTN3N]Mo(N2), where [HIPTN3N]3– is [{3,5-(2,4,6-i-Pr3C6H2)2C6H3NCH2CH2}3N]3–} in heptane. Slow addition of the proton source [{2,6-lutidinium}{BAr′4}, where Ar′ is 3,5-(CF3)2C6H3]and reductant (decamethyl chromocene) was critical for achieving high efficiency (∼66% in four turnovers). Numerous x-ray studies, along with isolation and characterization of six proposed intermediates in the catalytic reaction under noncatalytic conditions, suggest that N2 was reduced at a sterically protected, single molybdenum center that cycled from Mo(III) through Mo(VI) states.

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