Synthesis of 3,3-oxaspirocycles via cobalt-catalyzed cascade C-H activation and carboamidation of alkynes

Spirocyclic motifs are increasingly recognized as privileged scaffolds in drug discovery due to their unique three-dimensional architecture and favorable pharmacokinetic properties. Despite significant progress in the synthesis of carbo- and hetero-spirocycles, efficient methods for constructing oxa-spirocyclic frameworks remain underdeveloped. We present a one-step, cobalt(III)-catalyzed protocol for the synthesis of oxa-spirocyclic compounds using phenoxy acetamide and alkynes. The reaction is highly versatile, accommodating a range of functional groups on the aromatic ring and providing spirocyclic products in good to excellent yields. Substitutions at the quinone ring or internal alkyne prevent further cyclization, leading exclusively to the 1,2-carboamidated product. The carboamidation protocol is extended to unactivated olefins, and the subsequent acid-mediated post-synthetic modifications allow for the generation of complex three-dimensional structures. Kinetic studies and DFT calculations identify migratory insertion as the rate-determining step, with acetic acid assisting in the oxidative addition of the N-O bond and protodemetalation. This work provides a robust and efficient strategy for synthesizing oxa-spirocyclic compounds, showcasing the potential of cobalt(III) catalysis in complex molecular synthesis.

Authors

Institutions

Publication Details

Journal
Communications Chemistry
Published
2025-07-05
DOI
https://doi.org/10.1038/s42004-025-01580-5
Citations
2
Primary Topic
Catalytic C–H Functionalization Methods
Type
article
Field-Weighted Citation Impact
1.87

Funders

Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Synthesis of 3,3-oxaspirocycles via cobalt-catalyzed cascade C-H activation and carboamidation of alkynes

Bholanath Garai, Basker Sundararaju, Molla Rahamat Ali, J. Richard Premkumar
2 citations
Communications Chemistry
Catalytic C–H Functionalization Methods
1.87
article

Synthesis of 3,3-oxaspirocycles via cobalt-catalyzed cascade C-H activation and carboamidation of alkynes

Bholanath Garai, Basker Sundararaju, Molla Rahamat Ali, J. Richard Premkumar
article en
2 citations

Abstract

Spirocyclic motifs are increasingly recognized as privileged scaffolds in drug discovery due to their unique three-dimensional architecture and favorable pharmacokinetic properties. Despite significant progress in the synthesis of carbo- and hetero-spirocycles, efficient methods for constructing oxa-spirocyclic frameworks remain underdeveloped. We present a one-step, cobalt(III)-catalyzed protocol for the synthesis of oxa-spirocyclic compounds using phenoxy acetamide and alkynes. The reaction is highly versatile, accommodating a range of functional groups on the aromatic ring and providing spirocyclic products in good to excellent yields. Substitutions at the quinone ring or internal alkyne prevent further cyclization, leading exclusively to the 1,2-carboamidated product. The carboamidation protocol is extended to unactivated olefins, and the subsequent acid-mediated post-synthetic modifications allow for the generation of complex three-dimensional structures. Kinetic studies and DFT calculations identify migratory insertion as the rate-determining step, with acetic acid assisting in the oxidative addition of the N-O bond and protodemetalation. This work provides a robust and efficient strategy for synthesizing oxa-spirocyclic compounds, showcasing the potential of cobalt(III) catalysis in complex molecular synthesis.

Communications ChemistryVol. 8(1)
Holy Cross College (GB), Indian Institute of Technology Kanpur (IN)
Indian Institute of Technology Kanpur, Science and Engineering Research Board
Openalex Percentile: Top 15%
Catalytic C–H Functionalization Methods
1.87
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.

Synthesis of 3,3-oxaspirocycles via cobalt-catalyzed cascade C-H activation and carboamidation of alkynes — Bholanath Garai, Basker Sundararaju, et al. · Communications Chemistry (2025) | TGRS Research Map | TGRS