Elucidation of the biosynthesis of the methane catalyst coenzyme F(430).
Elucidation of the biosynthesis of the methane catalyst coenzyme F(430).
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DOI：
10.1038/nature21427
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发表时间：
2017-03-02
期刊：
影响因子：
64.8
通讯作者：
Warren MJ
中科院分区：
文献类型：
--
作者：
Moore SJ;Sowa ST;Schuchardt C;Deery E;Lawrence AD;Ramos JV;Billig S;Birkemeyer C;Chivers PT;Howard MJ;Rigby SE;Layer G;Warren MJ
甲烷生物发生在甲烷剂中是由甲基辅酶M还原酶介导的，这是一种酶，该酶也是通过厌氧甲烷氧化来利用甲烷的酶。该酶采用称为辅酶F430的辅助因子，这是一种含镍的修饰的四吡咯，通过新型甲基自由基/Ni（II） - 硫醇酸盐中间体促进催化。然而，尽管该途径必须涉及螯合，脑部降低，乳清环还原，乳杆菌和碳纤维环状形成，但共同原始子尿形成肌F430的生物合成F430（将11个空间中心纳入大环中）仍然很差。现在，我们已经确定了催化菌酶F430生物合成的蛋白质，称为CFBA-E，并显示其活性。这项研究完成了我们对自然如何能够构建基于四吡咯的生命色素的曲目的理解，从而使重组系统的开发更广泛地利用这些金属植物群。
Methane biogenesis in methanogens is mediated by methyl-coenzyme M reductase, an enzyme that is also responsible for the utilisation of methane through anaerobic methane oxidation. The enzyme employs an ancillary factor called coenzyme F430, a nickel-containing modified tetrapyrrole that promotes catalysis through a novel methyl radical/Ni(II)-thiolate intermediate. However, the biosynthesis of coenzyme F430 from the common primogenitor uroporphyrinoge III, incorporating 11 steric centres into the macrocycle, has remained poorly understood although the pathway must involve chelation, amidation, macrocyclic ring reduction, lactamisation and carbocyclic ring formation. We have now identified the proteins that catalyse coenzyme F430 biosynthesis from sirohydrochlorin, termed CfbA-E, and shown their activity. The research completes our understanding of how nature is able to construct its repertoire of tetrapyrrole-based life pigments, permitting the development of recombinant systems to utilise these metalloprosthetic groups more widely.