An ew catalytic system for the N-monoalkylation of aqueous ammonia with av ariety of alcohols was developed. Water-soluble dicationic complexes of iridium bearingN -heterocyclic carbene andd iammine ligands exhibited high catalytic activity for this type of reaction on the basis of hydrogen-transferp rocesses without generating harmfulo rw asteful byproducts. Various primary amines were efficiently synthesized by using safe, inexpensive, and easily handled aqueous ammonia as an itrogen source.F or example, the reaction of 1-(4-methylphenyl)ethanol with aqueous ammonia in the presence of aw ater-soluble Nheterocyclic carbene complexo fi ridium at 150 8Cf or 40 h gave 1-(4-methylphenyl)ethylamine in 83 %yield.Scheme1.Selective catalytic synthesis of primarya mines by N-alkylation of ammonia with alcohols.[a] Prof.