Divergent CH Insertion–Cyclization Cascades of <i>N</i>‐Allyl Ynamides

Holly V. Adcock, Elli Chatzopoulou, Paul Davies

Angewandte Chemie International Edition · 2015 · 80 citations · 75 references

DOIFull text

Open access

Concepts

Abstract

Gold carbene reactivity patterns were accessed by ynamide insertion into a C(sp(3) )H bond. A substantial increase in molecular complexity occurred through the cascade polycyclization of N-allyl ynamides to form fused nitrogen-heterocycle scaffolds. Exquisite selectivity was observed despite several competing pathways in an efficient gold-catalyzed synthesis of densely functionalized C(sp(3) )-rich polycycles and a copper-catalyzed synthesis of fused pyridine derivatives. The respective gold-keteniminium and ketenimine activation pathways have been explored through a structure-reactivity study, and isotopic labeling identified turnover-limiting CH bond-cleavage in both processes.

References

75