5 years ago

Reduction of Dinitrogen to Ammonia Catalyzed by Molybdenum Diamido Complexes

Reduction of Dinitrogen to Ammonia Catalyzed by Molybdenum Diamido Complexes
Takaya Ogawa, Lasantha A. Wickramasinghe, Peter Müller, Richard R. Schrock
[Ar2N3]Mo(N)(O-t-Bu), which contains the conformationally rigid pyridine-based diamido ligand, [2,6-(ArNCH2)2NC5H3]2– (Ar = 2,6-diisopropylphenyl), can be prepared from H2[Ar2N3], butyllithium, and (t-BuO)3Mo(N). [Ar2N3]Mo(N)(O-t-Bu) serves as a catalyst or precursor for the catalytic reduction of molecular nitrogen to ammonia in diethyl ether between −78 and 22 °C in a batchwise manner with CoCp*2 as the electron source and Ph2NH2OTf as the proton source. Up to ∼10 equiv of ammonia can be formed per Mo with a maximum efficiency in electrons of ∼43%.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b04800

DOI: 10.1021/jacs.7b04800

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