Hydroamination of alkenes with dinitrogen in a trititanium polyhydride framework

Abstract

The direct use of abundant and easily accessible molecules such as dinitrogen (N2) and alkenes as feedstocks for the synthesis of alkyl amines1 is of great interest and importance but remains a challenge2,3,4. Typically, N2 functionalization requires electrophilic carbon sources to facilitate the C‒N bond formation. Here we report hydroamination of nonactivated alkenes with N2 at a trititanium hydride framework, which can serve as an excellent platform for the activation of both alkenes and N2 and lead to selective C‒N bond formation between these two substrates, efficiently affording the corresponding alkyl amines upon further hydrogenation and protonation. Computational studies reveal the mechanistic details of N2 activation and selective C‒N bond formation. This work demonstrates a new strategy for transformation of N2 and simple hydrocarbons into nitrogen-containing organic compounds mediated by multinuclear hydride frameworks.