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Stoichiometric reduction of N2 at a Mo center stabilized by a bulky tetradentate phosphine ligand (${{\rm PP}{{{\rm Cy}\hfill \atop 3\hfill}}}$) allowed isolation of Mo–imidoamine and Mo–imido complexes. Both complexes as well as the MoII precursor are equally suitable catalysts for the synthesis of NTMS3 (TMS=trimethylsilyl) from N2, TMSCl, and electron sources. Mechanistic studies prove the involvement...
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