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Synthesis and Reactivity of a Zinc Diazoalkyl Complex: [3+2] Cycloaddition Reaction with Carbon Monoxide

Shengjie Jiang, Yanping Cai, Thayalan Rajeshkumar, Iker Del Rosal, Laurent Maron, Xin Xu

2023Angewandte Chemie International Edition18 citationsDOI

Abstract

Abstract This work reports the synthesis, characterization, and reactivity of the first example of a well‐defined zinc α‐diazoalkyl complex. Treatment of zinc(I)‐zinc(I) bonded compound L 2 Zn 2 [ L =CH 3 C(2,6‐ i Pr 2 C 6 H 3 N)CHC(CH 3 )(NCH 2 CH 2 PPh 2 )] or zinc(II) hydride L ZnH with trimethylsilyldiazomethane affords zinc diazoalkyl complex L ZnC(N 2 )SiMe 3 . This complex liberates N 2 in the presence of a nickel catalyst to form an α‐zincated phosphorus ylide by reacting with the pendant phosphine. It selectively undergoes formal [3+2] cycloaddition with CO 2 or CO to form the corresponding product with a five‐membered heterocyclic core. Notably, the use of CO in such a [3+2] cycloaddition reaction is unprecedented, reflecting a novel CO reaction mode.

Topics & Concepts

CycloadditionZincChemistryPhosphineReactivity (psychology)Carbon monoxideYlideCatalysisMedicinal chemistryHydrideNickelPolymer chemistryOrganic chemistryHydrogenPathologyMedicineAlternative medicineCyclopropane Reaction MechanismsN-Heterocyclic Carbenes in Organic and Inorganic ChemistryOrganometallic Complex Synthesis and Catalysis