Iron-Catalyzed Reductive Coupling of Alkyl Iodides with Alkynes To Yield cis-Olefins: Mechanistic Insights from Computation

被引:18
作者
Daru, Andrea [1 ]
Hu, Xile [2 ]
Harvey, Jeremy N. [1 ]
机构
[1] Katholieke Univ Leuven, Div Quantum Chem & Phys Chem, Dept Chem, Celestijnenlaan 200F, B-3001 Leuven, Belgium
[2] Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Inorgan Synth & Catalysis, ISIC LSCI, BCH 3305, CH-1015 Lausanne, Switzerland
基金
欧盟地平线“2020”;
关键词
CORRELATED MOLECULAR CALCULATIONS; GAUSSIAN-BASIS SETS; SPIN-CROSSOVER; REACTIVITY; COMPLEXES; KINETICS; HALIDES; CHEMISTRY; ENERGY; HYDROGENATION;
D O I
10.1021/acsomega.9b03578
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In a recent study, a new procedure for Z-selective olefin synthesis by reductive coupling of alkyl iodides with terminal alkynes in the presence of iron salts is described. This transformation is representative of many newly developed synthetic routes through the involvement of multiple species and phases, which makes mechanistic insight hard to obtain. Here, we report computational work aimed at exploring the possible reaction pathways. DFT calculations lead to two suggested routes, one involving C-I reduction by metallic zinc and radical addition to the alkyne and the other involving addition of two reduced iron species to the alkyne bond followed by reductive elimination. Comparison to experimental results as well as kinetic modeling is used to discuss the likelihood of these and related mechanisms.
引用
收藏
页码:1586 / 1594
页数:9
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