High‐Valent Nickel Complexes Supported by a Functionalized PC( sp 3 )P Pincer Ligand: Properties and Catalysis

Abstract This article presents the synthesis and characterization of a series of robust high‐valent organometallic nickel (Ni) complexes stabilized by a functionalized PC(sp 3 )P pincer ligand. Notably, the nickel center, covalently confined within the 3D ligand framework, demonstrates predictable coordination and redox behavior, coupled with remarkable stability across oxidation states +2, +3, and +4. These states were found to interconvert via one‐electron transfer reactions. Among these complexes, the Ni(III)‐PC(sp 3 )P species was identified as an efficient catalyst for the mild and selective hydrosilylation of alkenes, operating through a nonoxidative reaction mechanism.