Hydrogen Activation with Ru-PN3P Pincer Complexes for the Conversion of C1 Feedstocks

• DOI: 10.1021/acs.inorgchem.3c04001
• Publication Date: 2024-02-08T23:08:56Z
• Authors: Matthew D. Morton; Boon Ying Tay; Justin J.Q. Mah; Andrew J.P. White; James D. Nobbs; Martin van Meurs; George J.P. Brito...

The hydrogenation of C1 feedstocks (CO and CO2) has been investigated using ruthenium complexes [RuHCl(CO)(PN3P)] as the catalyst. PN3P pincer ligands containing amines in linker between central pyridine donor phosphorus donors with bulky substituents (tert-butyl (1) or TMPhos (2)) are required to obtain mononuclear single-site catalysts that can be activated by addition KOtBu generate stable five-coordinate [RuH(CO)(PN3P–H)], whereby ligand deprotonated. Activation hydrogen takes place via heterolytic cleavage [RuH2(CO)(PN3P)], but presence CO, coordination CO occurs preferentially give [RuH(CO)2(PN3P–H)]. This complex protonated cationic [RuH(CO)2(PN3P)]+, it is unable activate H2 heterolytically. In case less coordinating CO2, both 1 2 highly efficient CO2 a base (DBU), which results TON 30,000 for formation formate.