Evaluating Molecular Cobalt Complexes for the Conversion of N₂ to NH₃
We report a molecular Co−N₂ complex that generates a greater-than-stoichiometric yield of NH₃ (>200% NH₃ per Co−N₂ precursor) via the direct reduction of N₂ with protons and electrons. A comparison of the featured Co−N₂ complex with structurally related Co−N₂ and Fe−N₂ species shows how remarkably sensitive the N₂ reduction performance of potential precatalysts is. As discussed, structural and electronic effects are relevant to Co/Fe−N₂ conversion activity, including π basicity, charge state, and geometric flexibility.
© 2015 American Chemical Society. Received: March 24, 2015. Publication Date (Web): May 22, 2015. Special Issue: Small Molecule Activation: From Biological Principles to Energy Applications. This work was supported by the NIH (Grant GM 070757) and the Gordon and Betty Moore Foundation, and through the NSF via a GRFP award to T.J.D.C.
Supplemental Material - ic5b00645_si_001.pdf
Supplemental Material - ic5b00645_si_002.cif
Accepted Version - nihms726070.pdf