Affiliation:
1. Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
Abstract
Dinitrogen (N
2
) is reduced to ammonia at room temperature and 1 atm with molybdenum catalysts that contain tetradentate [HIPTN
3
N]
3−
triamidoamine ligands {[HIPTN
3
N]
3−
=[{3,5-(2,4,6-
i
-Pr
3
C
6
H
2
)
2
C
6
H
3
NCH
2
CH
2
}
3
N]
3−
, an example being [HIPTN
3
N]Mo(N
2
)} in heptane. Slow addition of the proton source ({2,6-lutidinium}{BAr′
4
}; Ar′=3,5-(CF
3
)
2
C
6
H
3
) and reductant (decamethyl chromocene) assure a high yield of ammonia (63–65% in four turnovers) versus dihydrogen formation. Numerous X-ray studies, along with isolation and characterization of seven intermediates in the proposed catalytic reaction (under noncatalytic conditions), suggest that N
2
is being reduced at a sterically protected, single Mo centre that cycles between states Mo(III), Mo(IV), Mo(V) and Mo(VI).
Subject
General Physics and Astronomy,General Engineering,General Mathematics
Cited by
35 articles.
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