A Fluorination/Aryl Migration/Cyclization Cascade for the Metal-Free Synthesis of Fluoro-Benzoxazepines

被引:72
|
作者
Ulmer, Anna [1 ,2 ]
Brunner, Christoph [1 ,2 ]
Arnold, Andreas M. [1 ,2 ]
Poethig, Alexander [1 ,2 ]
Gulder, Tanja [1 ,2 ]
机构
[1] Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85747 Garching, Germany
[2] Tech Univ Munich, Catalysis Res Ctr, Lichtenbergstr 4, D-85747 Garching, Germany
关键词
1; 2-aryl shift; benzoxazepines; fluorination; hypervalent iodine; ONE-POT SYNTHESIS; IODOTOLUENE DIFLUORIDE; HYPERVALENT; REARRANGEMENTS; REAGENTS; FLUOROCYCLIZATION; OXYFLUORINATION; DESIGN; ROUTE; SALTS;
D O I
10.1002/chem.201504749
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Fluorinated organic molecules are of high interest for many applications across chemical and medical disciplines. Efficient methods for the synthesis of such compounds are thus needed. Within this work, application of the bench-stable cyclic hypervalent iodine(III) fluoro reagent 1 facilitated the development of an efficient, metal-free method for the preparation of the novel class of 4-fluoro-1,3-benzoxazepines starting from readily available styrenes. The efficacy and broad applicability of this concept is demonstrated by the synthesis of 20 structurally diverse congeners in high yields, regio-, and diastereoselectivities. The presented method provides complementary chemoselectivity when compared to the common, commercially available electrophilic fluorination reagents, such as selectfluor. First mechanistic investigations with isotopically labeled substrates reveal a complex reaction mechanism, proceeding via an unusual fluorination/1,2-aryl migration/cyclization cascade.
引用
收藏
页码:3660 / 3664
页数:5
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