Zeng Yibin, Smith Brenton T, Hershberger John, Aubé Jeffrey
Department of Medicinal Chemistry, 1251 Wescoe Hall Drive, Room 4070, Malott Hall, University of Kansas, Lawrence, Kansas 66045-7852, USA.
J Org Chem. 2003 Oct 17;68(21):8065-7. doi: 10.1021/jo035004b.
The rearrangement of nitrones to lactams can be carried out by photochemical activation or by treatment with Tf(2)O followed by KOH-promoted rearrangement (a modification of conditions originally introduced by Barton). Substrates in which the nitrone is part of a fused bicyclic ring system have traditionally proven problematic for this kind of reaction. In this study, a series of mono-, bi-, and tricyclic ring-fused nitrones were prepared to investigate the dependence of products on nitrone ring size and tether length. Results indicated that photochemical rearrangement of nitrones in benzene afforded reasonably good yields (30-68%) of lactams, while the two-step nonphotochemical process provided slightly better average yields (30-95%) of the same targets.
硝酮重排为内酰胺可通过光化学活化或用三氟甲磺酸酐(Tf(2)O)处理,随后进行氢氧化钾促进的重排反应(这是对巴顿最初提出的条件的一种改进)来实现。传统上已证明,对于此类反应,硝酮作为稠合双环体系一部分的底物存在问题。在本研究中,制备了一系列单环、双环和三环稠合硝酮,以研究产物对硝酮环大小和连接链长度的依赖性。结果表明,在苯中进行硝酮的光化学重排可得到产率相当不错(30 - 68%)的内酰胺,而两步非光化学过程能为相同目标产物提供略高的平均产率(30 - 95%)。