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A suicide enzyme catalyzes multiple reactions for biotin biosynthesis in cyanobacteria
Nature Chemical Biology ( IF 12.9 ) Pub Date : 2020-02-10 , DOI: 10.1038/s41589-019-0461-9
Kei Sakaki 1 , Keita Ohishi 1 , Tetsu Shimizu 1 , Ikki Kobayashi 2 , Naoki Mori 3 , Kenichi Matsuda 1 , Takeo Tomita 1, 4 , Hidenori Watanabe 3 , Kan Tanaka 2 , Tomohisa Kuzuyama 1, 4 , Makoto Nishiyama 1, 4
Affiliation  

In biotin biosynthesis, the conversion of pimeloyl intermediates to biotin is catalyzed by a universal set of four enzymes: BioF, BioA, BioD and BioB. We found that the gene homologous to bioA, the product of which is involved in the conversion of 8-amino-7-oxononanoate (AON) to 7,8-diaminononanoate (DAN), is missing in the genome of the cyanobacterium Synechocystis sp. PCC 6803. We provide structural and biochemical evidence showing that a novel dehydrogenase, BioU, is involved in biotin biosynthesis and functionally replaces BioA. This enzyme catalyzes three reactions: formation of covalent linkage with AON to yield a BioU-DAN conjugate at the ε-amino group of Lys124 of BioU using NAD(P)H, carboxylation of the conjugate to form BioU-DAN-carbamic acid, and release of DAN-carbamic acid using NAD(P)+. In this biosynthetic pathway, BioU is a suicide enzyme that loses the Lys124 amino group after a single round of reaction.



中文翻译:

一种自杀酶催化蓝藻生物素生物合成的多种反应

在生物素生物合成中,庚二酰中间体向生物素的转化由一组通用的四种酶催化:BioF、BioA、BioD 和 BioB。我们发现与bioA同源的基因在蓝藻集胞藻的基因组中缺失,该基因的产物涉及 8-氨基-7-氧壬酸 (AON) 到 7,8-二氨基壬酸 (DAN) 的转化。sp。PCC 6803. 我们提供的结构和生化证据表明,一种新型脱氢酶 BioU 参与了生物素的生物合成并在功能上取代了 BioA。该酶催化三个反应:与 AON 形成共价键,使用 NAD(P)H 在​​ BioU 的 Lys124 的 ε-氨基处产生 BioU-DAN 偶联物,偶联物羧化形成 BioU-DAN-氨基甲酸,和使用 NAD(P) +释放 DAN-氨基甲酸。在这种生物合成途径中,BioU 是一种自杀酶,在单轮反应后会失去 Lys124 氨基。

更新日期:2020-02-10
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