The catalytic reduction of dinitrogen to ammonia with protons and electrons has been a key phenomenon in current developments of nitrogen fixation. In support, we have studied the synthesis of a rigid and acid stable long lived catalyst contains Calix[6]areneTren (L) ligand framework. Insertion of molybdenum to tren-based triamidoamine3- ligand has produced a C3v symmetric MoN complex, where Mo occupied in a tetradentate apical pocket. CAC(OMe)6Tren-MoN and CAC(OMe)3(H)3Tren-MoN have been prepared from triply deprotonated ligand (L3-) reacting with MoN(t-BuO)3. These Mo-complexes have shown a greater resistance toward ligand protonation under the conditions employed in catalysis. Characterizations were done by NMR spectroscopy and X-ray crystallography. Catalytic N2 reduction has been investigated using various proton and electron sources such as Ph2NH2OTf, H(Et2O)2Barf (Barf= [B(3,5-(CF3)2C6H3)4]), KC8 CoCp*2. These studies reveal more information leading to understand the importance of structural rigidity and reactivity in catalytic dinitrogen reduction.

Syntheses of structurally rigid Mo-Calix[6]azacryptand complexes and studies of dinitrogen reduction

256th National Meeting (2018)

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