Ammonia Synthesis by Hydrogenolysis of Titanium–Nitrogen Bonds Using Proton Coupled Electron Transfer | Zendy

Iraklis Pappas | Zendy; Paul J. Chirik | Zendy

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Ammonia Synthesis by Hydrogenolysis of Titanium–Nitrogen Bonds Using Proton Coupled Electron Transfer

Author(s) -

Iraklis Pappas,

Paul J. Chirik

Publication year - 2015

Publication title -

journal of the american chemical society

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 7.115

H-Index - 612

eISSN - 1520-5126

pISSN - 0002-7863

DOI - 10.1021/jacs.5b01047

Subject(s) - chemistry , hydrogenolysis , catalysis , ammonia , amide , dissociation (chemistry) , hydride , inorganic chemistry , electron transfer , rhodium , homolysis , photochemistry , metal , organic chemistry , radical

The catalytic hydrogenolysis of the titanium-amide bond in (η(5)-C5Me4SiMe3)2Ti(Cl)NH2 to yield free ammonia is described. The rhodium hydride, (η(5)-C5Me5)(py-Ph)RhH (py-Ph = 2-phenylpyridine), serves as the catalyst and promotes N-H bond formation via hydrogen atom transfer. The N-H bond dissociation free energies of ammonia ligands have also been determined for titanocene and zirconocene complexes and reveal a stark dependence on metal identity and oxidation state. In all cases, the N-H BDFEs of coordinated NH3 decreases by >40 kcal/mol from the value in the free gas phase molecule.

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