Formaldehyde formation in the glycine cleavage system and its use for an aldolase-based biosynthesis of 1,3-prodanediol

文献类型： 外文期刊

第一作者： Xu, Yingying

作者： Xu, Yingying;Meng, Hao;Zeng, An-Ping;Ren, Jie;Zeng, An-Ping

作者机构：

关键词： Glycine cleavage system; Formaldehyde; 5; 10-CH2-THF; 1; 3; propanediol

期刊名称：JOURNAL OF BIOLOGICAL ENGINEERING （ 影响因子：4.355； 五年影响因子：5.189 ）

ISSN： 1754-1611

年卷期： 2020 年 14 卷 1 期

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收录情况： SCI

摘要： Glycine cleavage system (GCS) occupies a key position in one-carbon (C1) metabolic pathway and receives great attention for the use of C1 carbons like formate and CO2 via synthetic biology. In this work, we demonstrate that formaldehyde exists as a substantial byproduct of the GCS reaction cycle. Three causes are identified for its formation. First, the principal one is the decomposition of N-5,N-10-methylene-tetrahydrofolate (5,10-CH2-THF) to form formaldehyde and THF. Increasing the rate of glycine cleavage promotes the formation of 5,10-CH2-THF, thereby increasing the formaldehyde release rate. Next, formaldehyde can be produced in the GCS even in the absence of THF. The reason is that T-protein of the GCS can degrade methylamine-loaded H-protein (H-int) to formaldehyde and ammonia, accompanied with the formation of dihydrolipoyl H-protein (H-red), but the reaction rate is less than 0.16% of that in the presence of THF. Increasing T-protein concentration can speed up the release rate of formaldehyde by H-int. Finally, a certain amount of formaldehyde can be formed in the GCS due to oxidative degradation of THF. Based on a formaldehyde-dependent aldolase, we elaborated a glycine-based one carbon metabolic pathway for the biosynthesis of 1,3-propanediol (1,3-PDO) in vitro. This work provides quantitative data and mechanistic understanding of formaldehyde formation in the GCS and a new biosynthetic pathway of 1,3-PDO.

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