Tyler Jasper L, Noble Adam, Aggarwal Varinder K
School of Chemistry, University of Bristol, Cantock's Close, Bristol, BS8 1TS, UK.
Angew Chem Int Ed Engl. 2021 May 17;60(21):11824-11829. doi: 10.1002/anie.202102754. Epub 2021 Apr 16.
Due to their intrinsic rigidity, three-dimensionality and structural novelty, spirocyclic molecules have become increasingly sought-after moieties in drug discovery. Herein, we report a strain-release driven synthesis of azetidine-containing spirocycles by harnessing the inherent ring strain of the azabicyclo[1.1.0]butane (ABB) fragment. Novel ABB-ketone precursors bearing silyl-protected alcohols were synthesized in a single step and shown to engage in electrophile-induced spirocyclization-desilylation reactions. Primary, secondary and tertiary silyl ethers were effectively transformed into a library of new spiro-azetidines, with a range of substituents and ring sizes. In addition, the products are generated with synthetically useful ketone and protected-amine functional groups, which provides the potential for further elaboration and for this chemistry to be utilized in the rapid assembly of medicinally relevant compounds.
由于其固有的刚性、三维性和结构新颖性,螺环分子在药物发现中已成为越来越受追捧的基团。在此,我们报道了一种通过利用氮杂双环[1.1.0]丁烷(ABB)片段的固有环张力,实现含氮杂环丁烷螺环的应变释放驱动合成。带有硅基保护醇的新型ABB-酮前体可一步合成,并显示可参与亲电试剂诱导的螺环化-脱硅反应。伯、仲和叔硅基醚可有效地转化为一系列具有不同取代基和环大小的新型螺氮杂环丁烷文库。此外,产物生成了具有合成上有用的酮和保护胺官能团,这为进一步修饰以及将该化学方法用于快速组装与药物相关的化合物提供了潜力。