光酶式反选择性分子间基化
Xiaoqiang Huang1,2, Binju Wang3,4,5, Yajie Wang1,2
1Center for Advanced Bioenergy and Bioproducts Innovation, University of Illinois at Urbana-Champaign, Urbana, IL, USA.
Nature
|June 9, 2020
概括
这项研究引入了一种新型的酶催化反应,用于利用可见光光催化合成奇拉碳化合物. 该方法可实现高效的分子间基化,扩大生物催化应用.
科学领域:
- 生物催化和有机合成
- 光催化
- 酶工程
背景情况:
- 不对称合成中的酶应用受到自然发生的反应的限制.
- 光催化揭示了已知的酶的新反应性.
- 对分子间交叉合反应没有应用光诱导酶催化.
研究的目的:
- 开发一种新型的可见光诱导的分子间激素化,由缩酶催化.
- 用γ-立体中心合成奇拉性碳化合物.
- 克服酶光反应和立体化学控制方面的挑战.
主要方法:
- 使用""减少酶进行可见光诱导的基质化.
- 使用易于获得的α-碳酸化合物和终端基因作为基板.
- 通过基质-酶复合体的形成研究了机制性途径.
主要成果:
- 通过γ-立体中心实现了各种碳化合物的高效合成.
- 获得了优异的产量 (高达99%) 和反选择性 (高达99% ee).
- 证明了一种以前无法通过化学催化剂实现的方法.
结论:
- 开发的方法扩大了对不对称转换的生物催化反应能力.
- 光催化和酶催化的合并使得新的合成途径成为可能.
- 通过基质-酶复合体的形成触发了光选择性激素反应.
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