One-Step Construction of Atropisomers Bearing 1,5-Central and Axial Chirality via Catalytic Diastereo- and Atroposelective Remote Desymmetrizing Alkynylation
Catalytic asymmetric construction of atropisomers with multiple stereogenic elements has recently become an emerging area. However, general methods that produced atropisomers bearing remote 1,5-axial and central chirality efficiently and stereoselectively are scarce yet highly challenging. We herein report a catalytic diastereo- and atroposelective remote desymmetrizing alkynylation of axially prochiral dialkynes with ortho-quinone methides (o-QMs), furnishing atropisomers bearing 1,5-remote centrally and axially stereogenic elements. The remote control of prochiral axis far from the reaction site could be simultaneously achieved during the stereoselective C(sp3)–C(sp) bond-forming process to generate a stereogenic center. In addition, a kinetic resolution of axially racemic alkynes via diastereo- and atroposelective remote alkynylation with o-QMs has been developed, further enriching structural diversity of atropisomers bearing 1,5-central and axial chirality. The present method expands the chemical space of atropisomeric molecules bearing multiple chiral elements by facile downstream diversification of C–C triple bonds. Finally, the alkynylation of o-QMs can also be applied for the construction of chiral motifs bearing 1,9- and 1,10-stereogenic centers.
Authors
- Fangzhi Peng
- Kaixin Zhao (ORCID: https://orcid.org/0000-0002-0738-5930)
- Zhihui Shao (ORCID: https://orcid.org/0000-0003-4531-3417)
- Ming Jiang (ORCID: https://orcid.org/0000-0002-6426-4107)
- Yingcheng Wang (ORCID: https://orcid.org/0000-0002-1784-4504)
- Xiaoguang Li (ORCID: https://orcid.org/0000-0001-9979-053X)
- Shan Wang (ORCID: https://orcid.org/0000-0001-6565-1814)
- Zheng Wang (ORCID: https://orcid.org/0000-0002-7560-2618)
- Long Li (ORCID: https://orcid.org/0000-0002-0755-2751)
- Daming He (ORCID: https://orcid.org/0000-0002-9007-5545)
Institutions
- Shenzhen University (CN)
- Yunnan University (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2024-12-12
- DOI
- https://doi.org/10.1021/acscatal.4c06332
- Citations
- 7
- Primary Topic
- Axial and Atropisomeric Chirality Synthesis
- Type
- article
- Field-Weighted Citation Impact
- 1.75
Funders
- National Natural Science Foundation of China
- Major Science and Technology Projects in Yunnan Province