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‘ene’-Reductases for Asymmetric Carbonyl Desaturation

有机合成与工艺文献分享 2025-04-27 08:35
文章摘要
本文介绍了一种新型的不对称碳脱氢策略，通过揭示ene-reductases的反向催化活性，利用空气作为终端氧化剂，实现了对4,4′-二取代环己酮底物的对映选择性氧化，产率高达96%，对映体比例超过99:1。研究通过多轮进化获得了一系列突变体，优化条件下展示了超过50个实例的广泛底物范围，并耐受敏感官能团。此外，该策略在克级规模上验证了反应的对映选择性，并进一步应用于级联脱氢Michael加成或后续Diels−Alder和Babler−Dauben反应。机理分析揭示了突变体GkOYE3在脱氢反应的三个关键步骤中表现出增强的效率。
‘ene’-Reductases for Asymmetric Carbonyl Desaturation
查看文献： Unmasking the reverse catalytic activity of ‘ene’-reductases for asymmetric carbonyl desaturation
查看期刊：Nature chemistry
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