Photocatalytic Annulation of Primary Amines to δ-Lactams: Access to Privileged (Spiro)piperidine Space
Jacob C Turner-Dore1, Joseph J Bell-Tyrer1, Hannah E Askey1
1Department of Chemistry, University of Bath, Claverton Down, BathBA2 7AY, U.K.
Abstract:
Piperidines are the most prevalent saturated nitrogen heterocycles in pharmaceuticals, yet efficient and general methods for accessing α-disubstituted and spirocyclic variants have remained a long-standing synthetic challenge. A broadly applicable annulation strategy from unprotected primary alkylamines would represent an important advance, enabling access to privileged piperidine scaffolds from the most accessible nitrogen feedstocks. Here we disclose a general photoredox/hydrogen atom transfer dual catalytic annulation that converts primary amines into α-mono- and α-disubstituted δ-lactams, versatile intermediates that provide streamlined access to diverse piperidines. The method proceeds under mild conditions, can be scaled to ∼100 g in continuous flow, and affords products capable of downstream modification. This work provides a broadly applicable solution to a challenging problem in heterocycle synthesis, expanding the structural space accessible to drug discovery.
Related Concept Videos
Preparation of 1° Amines: Hofmann and Curtius Rearrangement Overview
Preparation of 1° Amines: Azide Synthesis
Azide ions act as good nucleophiles and react with unhindered alkyl halides to form alkyl azides. Alkyl azides do not participate in further nucleophilic substitution reactions, thereby eliminating the chances of polyalkylated products. Alkyl azides are reduced by hydride-based reducing agents, like lithium aluminum...
Preparation of 1° Amines: Hofmann and Curtius Rearrangement Mechanism
Acid Halides to Amides: Aminolysis
In the first step of the aminolysis mechanism, the amine attacks the carbonyl carbon of the acyl chloride to form a tetrahedral intermediate. In the second step, the carbonyl group is re-formed with the elimination of a chloride...
Preparation of 1° Amines: Gabriel Synthesis
Strong bases like NaOH or KOH deprotonate the phthalimide to form the corresponding anion, which acts as a nucleophile. Further, the anion attacks an...
Amines to Amides: Acylation of Amines
Next, the second equivalent of amine serves as a Brønsted base and deprotonates the quaternary amide...

![Cercosporin-Photocatalyzed [4+1]- and [4+2]-Annulations of Azoalkenes Under Mild Conditions](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F60786.jpg&w=3840&q=50)
![Solid-phase Synthesis of [4.4] Spirocyclic Oximes](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F58508.jpg&w=3840&q=50)