The study of Metal Ligand Cooperativity (MLC) and the reactivity of transition metals with non-innocent ligands is a flourishing field in organometallic chemistry. By pairing transformations at the metal center with those on the ligand, it is possible to achieve “apparent” reductive eliminations and oxidative additions that have no net change of the formal oxidation state of the metal center. MLC scaffolds have largely relied on nitrogen atoms to provide the redox active sites. Much less study has been conducted in this field with the next element in the pnictogen row: phosphorus. Herein, we report a triphosphorus ligand and its complexes of iridium (tBuPPHP)Ir(H)(Cl) and ruthenium (tBuPPHP)Ru(Cl)2. A pendant P-H bond on the bis-aryl phosphorus of this ligand allows it to coordinate as either a formally neutral or anionic ligand. This enables the phosphorus center to act as a “proton reservoir” for heterolytic cleavage of E-H (E = H, C, O, X) bonds. These complexes have shown reactivity towards various small molecules including ethylene and carbon monoxide. We are also investigating the capability of this ligand system to promote alkane dehydrogenation through heterolytic C-H activation across the P-M bond.

Phosphorus-based metal ligand cooperativity of iridium and ruthenium complexes. Synthesis, reactivity and catalytic efficacy

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.