AbnI: An α-ketoglutarate-dependent dioxygenase involved in brassicicene C-H functionalization and ring system rearrangement

AbnI: An α-ketoglutarate-dependent dioxygenase involved in brassicicene C-H functionalization and ring system rearrangement
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DOI:
10.1016/j.cclet.2023.108788
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发表时间:
2024-02-26
影响因子:
9.1
通讯作者:
Zhang,Yonghui
Zhang,Yonghui
中科院分区:
化学1区
文献类型:
--
作者:
Yuan,Wenling;Li,Fengli;Zhang,Yonghui

文献摘要

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我们报道了一个新的芸苔烯二萜生物合成基因簇的特征,该基因簇包含一个独特的α-酮戊二酸依赖性双加氧酶(αKGD),AbnI。我们的研究结果表明,AbnI表现出显着的底物混杂,并能够激活多个网站上的5-8-5和5-9-5芸苔素骨架,导致骨架的修改和一个意想不到的环系统重排。这些结果表明,潜在的效用AbnI作为一种酶的工具萜烯C单键H功能化。此外,还对AbnI的催化机制及其潜在的生态学意义进行了讨论。
We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster, which contains a uniqueα-ketoglutarate-dependent dioxygenase (αKGD) enzyme, AbnI. Our findings revealed that AbnI demonstrates remarkable substrate promiscuity and is capable of activating multiple sites on both 5–8–5 and 5–9–5 brassicicene skeletons, resulting in skeleton modifications and an unexpected ring system rearrangement. These results suggested the potential utility of AbnI as an enzymatic tool for terpene Csingle bondH functionalization. In addition, the catalytic mechanism of AbnI and its potential ecological implications were discussed.