Affiliation:
1. Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.
Abstract
Dinitrogen (N
2
) was reduced to ammonia at room temperature and 1 atmosphere with molybdenum catalysts that contain tetradentate [HIPTN
3
N]
3–
triamidoamine ligands {such as [HIPTN
3
N]Mo(N
2
), where [HIPTN
3
N]
3–
is [{3,5-(2,4,6-i-Pr
3
C
6
H
2
)
2
C
6
H
3
NCH
2
CH
2
}
3
N]
3–
} in heptane. Slow addition of the proton source [{2,6-lutidinium}{BAr′
4
}, where Ar′ is 3,5-(CF
3
)
2
C
6
H
3
]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 N
2
was reduced at a sterically protected, single molybdenum center that cycled from Mo(III) through Mo(VI) states.
Publisher
American Association for the Advancement of Science (AAAS)
Cited by
1270 articles.
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