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Stabilizing Doubly Deprotonated Diazomethane: Isolable Complexes with CN<sub>2</sub><sup>2–</sup> and CN<sub>2</sub><sup>–</sup> Radical Ligands

Ze‐Jie Lv, Philipp D. Engel, Lukas Alig, Sandipan Maji, Max C. Holthausen, Sven Schneider

2022Journal of the American Chemical Society21 citationsDOI

Abstract

Transition metal complexes with a doubly deprotonated diazomethane (CNN2–) ligand have been proposed as fleeting intermediates in nitrogen transfer reactions. However, in contrast to isoelectronic azide (N3–), well-defined examples are unknown. We here report the synthesis and characterization of isolable complexes with terminal and bridging CNN2– ligands, stabilized by platinum(II) pincer fragments. Bonding within the allenic dimetallanitrilimine core (Pt–N═N═C–Pt) was probed by oxidation of the bridging ligand. Enhanced reactivity toward [3 + 2]-cycloaddition with CO2 was obtained. Photofragmentation favors N–NC over NN–C bond cleavage as a route to cyanide and a transient metallonitrene complex.

Topics & Concepts

ChemistryDeprotonationDiazomethaneAzideLigand (biochemistry)Reactivity (psychology)CycloadditionCyanideBridging ligandStereochemistryPlatinumCarbeneBond cleavageMedicinal chemistryMetalPhotochemistryIonInorganic chemistryOrganic chemistryCatalysisMedicineAlternative medicineBiochemistryPathologyReceptorCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsCO2 Reduction Techniques and Catalysts
Stabilizing Doubly Deprotonated Diazomethane: Isolable Complexes with CN<sub>2</sub><sup>2–</sup> and CN<sub>2</sub><sup>–</sup> Radical Ligands | Litcius