A dual cellular–heterogeneous catalyst strategy for the production of olefins from glucose

A dual cellular–heterogeneous catalyst strategy for the production of olefins from glucose
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用于从葡萄糖生产烯烃的双细胞多相催化剂策略

DOI:
10.1038/s41557-021-00820-0
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发表时间:
2021
期刊:
影响因子:
21.8
通讯作者:
Chang, Michelle C.
Chang, Michelle C.
中科院分区:
化学1区
文献类型:
--
作者:
Wang, Zhen Q.;Song, Heng;Koleski, Edward J.;Hara, Noritaka;Park, Dae Sung;Kumar, Gaurav;Min, Yejin;Dauenhauer, Paul J.;Chang, Michelle C.

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生命系统为化学合成提供了一种很有前途的方法,它通过进化进行了优化,将可再生的碳源(如葡萄糖)转化为大量的小分子。然而,大量的合成结构仍然难以单独从细胞中获得,例如未取代的烃。在这项工作中,我们证明了使用一个双细胞多相催化策略,以产生烯烃从葡萄糖使用选择性水解酶,以产生一个活化的中间体,很容易脱氧。使用一种新的迭代硫解酶家族,我们对一种微生物菌株进行了基因工程改造,该菌株从葡萄糖中产生4.3 ± 0.4 g l− 1脂肪酸,其中86%被捕获为3-羟基辛酸和3-羟基癸酸。该3-羟基取代基用作离去基团,其使得能够在刘易斯酸性催化剂上进行非均相串联脱羧-脱水路线以得到烯烃产物,而无需简单脂肪酸的酶或化学脱氧所需的额外氧化还原输入。
Living systems provide a promising approach to chemical synthesis, having been optimized by evolution to convert renewable carbon sources, such as glucose, into an enormous range of small molecules. However, a large number of synthetic structures can still be difficult to obtain solely from cells, such as unsubstituted hydrocarbons. In this work, we demonstrate the use of a dual cellular–heterogeneous catalytic strategy to produce olefins from glucose using a selective hydrolase to generate an activated intermediate that is readily deoxygenated. Using a new family of iterative thiolase enzymes, we genetically engineered a microbial strain that produces 4.3 ± 0.4 g l−1of fatty acid from glucose with 86% captured as 3-hydroxyoctanoic and 3-hydroxydecanoic acids. This 3-hydroxy substituent serves as a leaving group that enables heterogeneous tandem decarboxylation–dehydration routes to olefinic products on Lewis acidic catalysts without the additional redox input required for enzymatic or chemical deoxygenation of simple fatty acids.
钨(Vi)配合物催化β-羟基羧酸转化为烯烃:一种新型酰基转移催化剂
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