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A new asymmetric chiral PNP ligand based on the 2,6-diaminopyridine scaffold featuring a R -BINEPINE moiety was prepared. Treatment of anhydrous FeX 2 (X = Cl, Br) with 1 equiv of PNP- i Pr,BIN at room temperature afforded the coordinatively unsaturated paramagnetic complexes [Fe(PNP- i Pr,BIN)X 2 ]. The structure of [Fe(PNP- i Pr,BIN)Cl 2 ] is described. Both complexes react readily with the strong π-acceptor ligand CO in solution to afford selectively the diamagnetic complexes trans -[Fe(PNP- i Pr,BIN)(CO)X 2 ] in quantitative yield. Due the lability of the CO ligand, these complexes are only stable under a CO atmosphere and isolation in pure form was not possible. The preparation of the carbonyl hydride complex [Fe(PNP- i Pr,BIN)(H)(CO)Br] was achieved albeit in low yields via a one pot procedure by treatment of [Fe(PNP- i Pr,BINEP)Br 2 ] with CO and subsequent reaction with Na[HBEt 3 ]. This complex was obtained as an inseparable mixture of two diastereomers in a ca. 1:1 ratio and was tested as catalyst for the hydrogenation of ketones. The catalyst showed acceptable activity under mild conditions (5 bar H 2 , room temperature) with yields up to &gt;99 % within 18 h.

Synthesis and reactivity of BINEPINE-based chiral Fe(II) PNP pincer complexes