Journal
CHEMICAL SCIENCE
Volume 13, Issue 24, Pages 7310-7317Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1sc06986a
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Funding
- National Natural Science Foundation of China [21121062, 21302203, 21372250, 21772037, 21772226, 21861132014, 91956115, 22171078]
- Shanghai Municipal Science and Technology Major Project [2018SHZDZX03]
- Fundamental Research Funds for the Central Universities [222201717003]
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In this study, the mechanism of Rh(i) complex catalyzed dimerization of ene-vinylidenecyclopropanes was elucidated through experimental and computational studies, and a key intermediate was identified.
Rh(i) complex catalyzed dimerization of ene-vinylidenecyclopropanes took place smoothly to construct a series of products containing spiro[4,5]decane skeletons featuring a simple operation procedure, mild reaction conditions, and good functional group tolerance. In this paper, the combination of experimental and computational studies reveals a counterion-assisted Rh(i)-Rh(iii)-Rh(v)-Rh(iii)-Rh(i) catalytic cycle involving tandem oxidative cyclometallation/reductive elimination/selective oxidative addition/selective reductive elimination/reductive elimination steps; in addition, a pentavalent spiro-rhodium intermediate is identified as the key intermediate in this dimerization reaction upon DFT calculation.
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