Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 103, Issue 46, Pages 17099-17106Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0602778103
Keywords
catalysis; fixation; nitrogenase
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Funding
- NIGMS NIH HHS [R01 GM031978, GM 31978] Funding Source: Medline
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Since our discovery of the catalytic reduction of dinitrogen to ammonia at a single molybdenum center, we have embarked on a variety of studies designed to further understand this complex reaction cycle. These include studies of both individual reaction steps and of ligand variations. An important step in the reaction sequence is exchange of ammonia for dinitrogen in neutral molybdenum(III) compounds. We have found that this exchange reaction is first order in dinitrogen and relatively fast (complete in < 1 h) at 1 atm of dinitrogen. Variations of the terphenyl substituents in the triamicloamine ligand demonstrate that the original ligand is not unique in its ability to yield successful catalysts. However, complexes that contain sterically less demanding ligands fail to catalyze formation of ammonia from dinitrogen; it is proposed as a consequence of a base-catalyzed decomposition of a diazeniclo (Mo-N=NH) intermediate.
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