饱和突变
化学
生物催化
立体化学
突变
醛缩酶A
立体专一性
苯甲醛
生物化学
组合化学
酶
部分
氯霉素
分子模型
立体异构
蛋白质工程
异构化
活动站点
丙氨酸
立体选择性
分子动力学
生物合成
化学合成
氨基酸
氢键
动力学分辨率
作者
Shuya Sun,Yiquan Zhou,Feiyang Deng,Yifang Meng,Xinglu Zhu,Hualei Wang,Di Wei
标识
DOI:10.1021/acs.jafc.6c01578
摘要
l -Threonine aldolase (LTA) is an attractive biocatalyst for the synthesis of l - syn - p -nitrophenylserine ( l - syn -1b), a key intermediate in chloramphenicol synthesis. However, low diastereoselectivity has limited its broader application in stereospecific C–C bond formation. To overcome this limitation, a metagenomic library constructed from non-natural amino acid-enriched environments was screened, leading to the identification of an LTA from Staphylococcus epidermidis ( Se LTA) that exhibits the highest diastereoselectivity toward l - syn -1b among naturally occurring LTAs reported to date. To further enhance its diastereoselectivity, structural comparison, alanine scanning, and tunnel analysis were employed to identify hotspots that modulate the diastereoselectivity of Se LTA. Subsequent saturation mutagenesis and iterative saturation mutagenesis at these positions yielded the quadruple variant A176G/Y202S/N7C/F129E (Mut4), which increased the diastereoselectivity from 32.5% syn to 92.7% syn . Furthermore, Mut4 exhibits markedly improved diastereoselectivity toward para- and meta-substituted benzaldehyde derivatives. Molecular dynamics (MD) simulations further elucidated the molecular basis underlying the enhanced diastereoselectivity of Mut4. This study provides a potential biocatalyst for the sustainable and efficient synthesis of a chloramphenicol intermediate.
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