Orukotan Will E, Palate Kleopas Y, Pogrányi Balázs, Bobinski Philipp, Epton Ryan G, Duff Lee, Whitwood Adrian C, Grogan Gideon, Lynam Jason M, Unsworth William P
Department of Chemistry, University of York, York, YO10 5DD, UK.
Organisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 270, 69120, Heidelberg, Germany.
Chemistry. 2024 Feb 7;30(8):e202303270. doi: 10.1002/chem.202303270. Epub 2023 Dec 15.
Macrocyclic and medium-sized ring ketones, lactones and lactams can all be made from common acryloyl imide starting materials through divergent, one-pot cascade ring-expansion reactions. Following either conjugate addition with an amine or nitromethane, or osmium(VIII)-catalysed dihydoxylation, rearrangement through a four-atom ring expansion takes place spontaneously to form the ring expanded products. A second ring expansion can also be performed following a second iteration of imide formation and alkene functionalisation/ring expansion. In the dihydroxylation series, three- or four-atom ring expansion can be performed selectively, depending on whether the reaction is under kinetic or thermodynamic control.
大环和中环酮、内酯和内酰胺都可以由常见的丙烯酰亚胺起始原料通过发散性的一锅串联扩环反应制得。在与胺或硝基甲烷进行共轭加成,或锇(VIII)催化的二羟基化反应之后,会自发地通过四元环扩环进行重排,以形成扩环产物。在进行第二轮亚胺形成和烯烃官能化/扩环反应后,还可以进行第二次扩环。在二羟基化系列反应中,根据反应是处于动力学控制还是热力学控制,可以选择性地进行三元或四元环扩环。