Ru(II)-Triphos Catalyzed Amination of Alcohols with
Ammonia via Ionic Species
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Abstract
An active and selective system for
the amination of primary alcohols
to primary amines with ammonia based on ruthenium and triphos as the
tridentate phosphine ligand was developed. On the basis of detailed
mechanistic studies, we propose that the active catalyst is, unlike
the previously reported systems on this reaction, a cationic ruthenium
complex. The experimental findings are supported by detailed density
functional theory (DFT) calculations on the catalytic cycle. Because
of the cationic nature of the active catalyst, strong anion and solvent
effects were observed in the catalytic amination reaction when using
the ruthenium triphos complexes. Therefore, a higher activity could
be achieved when the nonpolar solvent toluene is used in this amination
instead of tetrahydrofuran. Our findings can help to develop and optimize
the system systematically for an application to relevant target molecules