1. Two-fold proton coupled electron transfer of a Ta(V) aniline complex mediated by a redox active NNN pincer ligand.
- Author
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Pavlidis, Sotirios, Alasadi, Jasmin, Opis-Basilio, Amanda, and Abbenseth, Josh
- Subjects
- *
ABSTRACTION reactions , *CHARGE exchange , *LIGANDS (Chemistry) , *DENSITY functional theory , *OXIDATION states - Abstract
We report the proton-coupled electron transfer (PCET) reactivity of an octahedral Ta(V) aniline complex supported by an acridane-derived redox active NNN pincer ligand. The reversible binding of aniline to a Ta(V) dichloride induces significant coordination-induced bond weakening (CIBW) of the aniline N–H bonds. This enables a rare two-fold hydrogen atom abstraction, resulting in a terminal imido complex and a two-electron oxidation of the NNN pincer ligand, all while maintaining the metal's oxidation state. The bond dissociation free energies (BDFEs) of the aniline and a transient radical amido complex are estimated through stoichiometric reactions with different hydrogen atom abstractors and donors, further supported by density functional theory calculations. [ABSTRACT FROM AUTHOR]
- Published
- 2025
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