Photoresponsive Aerobic Cross‐Dehydrogenative Coupling Reaction with Ammonium Iodide Catalyst

A photoresponsive aerobic cross‐dehydrogenative coupling reaction of N‐substituted tetrahydroisoquinolines with nitroalkanes using an iodide salt catalyst under blue LED irradiation is developed, furnishing the CC bond coupling products in high yields. Mechanistic studies indicate that the iodide salt catalyst promotes the single‐electron transfer from the N‐substituted tetrahydroisoquinolines to the nitroalkanes through the assembled tetrahydroisoquinoline–iodide salt complex to generate cation radicals of the tetrahydroisoquinolines under light irradiation.