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通过亚磺酰胺活化实现S(IV)-立体异构亚磺酰亚胺酯的不对称合成。

Asymmetric Synthesis of S(IV)-Stereogenic Sulfinimidate Esters by Sulfinamide Activation.

作者信息

Xiong Qiang, Liao Minghong, Zhao Sha, Wu Sitian, Hong Ya, Chi Yonggui Robin, Zhang Xinglong, Wu Xingxing

机构信息

State Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Guizhou University, Guiyang, 550025, China.

School of Chemistry, Chemical Engineering, and Biotechnology, Nanyang Technological University, Singapore, 637371, Singapore.

出版信息

Angew Chem Int Ed Engl. 2025 May;64(21):e202500170. doi: 10.1002/anie.202500170. Epub 2025 Mar 21.

Abstract

Catalyst-controlled approaches for the synthesis of S-stereogenic compounds have propelled significant advancements in asymmetric synthetic chemistry. In contrast, control over S-heteroatom (e.g., O) bond formation to access sulfinimidate esters remains an underexplored area. Drawing inspiration from recent progress in electrophilic amide activation, herein, we present a sulfinamide activation strategy for the enantioselective synthesis of S-chiral sulfinimidate esters. This method involves the activation of racemic sulfinamides by sulfonyl chloride, yielding a reactive aza-sulfinyl mixed anhydride intermediate. Employing a naturally occurring cinchonidine catalyst, the process achieves excellent enantiocontrol in the subsequent formation of S─O bonds with alcohols involving a dynamic kinetic resolution (DKR) process, resulting in sulfinimidate esters with excellent enantioselectivity. The catalytically obtained enantioenriched sulfinimidate esters offer a versatile platform for the construction of S-stereogenic frameworks, including sulfilimines and sulfoximines, with promising applications in asymmetric synthesis and drug discovery.

摘要

用于合成S-立体异构化合物的催化剂控制方法推动了不对称合成化学的重大进展。相比之下,通过控制S-杂原子(如O)键的形成来制备亚磺酰亚胺酯仍是一个未被充分探索的领域。借鉴亲电酰胺活化的最新进展,在此我们提出了一种用于对映选择性合成S-手性亚磺酰亚胺酯的亚磺酰胺活化策略。该方法涉及用磺酰氯活化外消旋亚磺酰胺,生成一种活性氮杂亚磺酰基混合酸酐中间体。使用天然存在的辛可尼定催化剂,该过程在随后与醇形成S─O键的过程中通过动态动力学拆分(DKR)实现了优异的对映体控制,从而得到具有优异对映选择性的亚磺酰亚胺酯。催化得到的对映体富集的亚磺酰亚胺酯为构建S-立体异构骨架提供了一个通用平台,包括亚磺酰亚胺和亚砜亚胺,在不对称合成和药物发现中具有广阔的应用前景。

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