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关于“末端过氧化物合酶 FtmOx1 催化机制的结构见解”的通信。

Correspondence on "Structural Insight into the Catalytic Mechanism of the Endoperoxide Synthase FtmOx1".

机构信息

State Key Laboratory of Bioreactor Engineering, East China University of Science and Technology, Shanghai, 200237, China.

College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China.

出版信息

Angew Chem Int Ed Engl. 2023 Sep 11;62(37):e202218643. doi: 10.1002/anie.202218643. Epub 2023 Aug 4.

DOI:10.1002/anie.202218643
PMID:37541669
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10528348/
Abstract

In their recent Angewandte Chemie publication (doi: 10.1002/anie.202112063), Cen, Wang, Zhou et al. reported the crystal structure of a ternary complex of the non-heme iron endoperoxidase FtmOx1 (PDB entry 7ETK). The biochemical data assessed in this study were from a retracted study (doi: 10.1038/nature15519) by Zhang, Liu, Zhang et al.; no additional biochemical data were included, yet there was no discussion on the source of the biochemical data in the report by Cen, Wang, Zhou et al. Based on this new crystal structure and subsequent QM/MM-MD calculations, Cen, Wang, Zhou et al. concluded that their work provided evidence supporting the CarC-like mechanistic model for FtmOx1 catalysis. However, the authors did not accurately describe either the CarC-like model or the COX-like model, and they did not address the differences between them. Further, and contrary to their interpretations in the manuscript, the authors' data are consistent with the COX-like model once the details of the CarC-like and COX-like models have been carefully analyzed.

摘要

在他们最近发表于《德国应用化学》的论文(doi:10.1002/anie.202112063)中,岑、王、周等人报道了非血红素铁过氧化物酶 FtmOx1 的三元复合物的晶体结构(PDB 条目 7ETK)。本研究评估的生化数据来自张、刘、张等人的一篇已撤回的研究(doi:10.1038/nature15519);研究中没有包含其他生化数据,但岑、王、周等人的报告中没有讨论生化数据的来源。基于这个新的晶体结构和随后的 QM/MM-MD 计算,岑、王、周等人得出结论,他们的工作为 FtmOx1 催化的 CarC 样机制模型提供了证据。然而,作者并没有准确描述 CarC 样模型或 COX 样模型,也没有讨论它们之间的差异。此外,与他们在稿件中的解释相反,一旦仔细分析了 CarC 样和 COX 样模型的细节,作者的数据就与 COX 样模型一致。

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本文引用的文献

1
Dissecting the Mechanism of the Nonheme Iron Endoperoxidase FtmOx1 Using Substrate Analogues.利用底物类似物剖析非血红素铁内过氧化物酶FtmOx1的作用机制。
JACS Au. 2022 Jun 10;2(7):1686-1698. doi: 10.1021/jacsau.2c00248. eCollection 2022 Jul 25.
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Structural Insight into the Catalytic Mechanism of the Endoperoxide Synthase FtmOx1.结构洞察过氧化物合酶 FtmOx1 的催化机制。
Angew Chem Int Ed Engl. 2022 Mar 14;61(12):e202112063. doi: 10.1002/anie.202112063. Epub 2022 Feb 3.
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Molecular insights into the endoperoxide formation by Fe(II)/α-KG-dependent oxygenase NvfI.
铁(II)/α-KG 依赖性加氧酶 NvfI 形成内过氧化物的分子见解。
Nat Commun. 2021 Jul 20;12(1):4417. doi: 10.1038/s41467-021-24685-6.
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Retraction Note: Endoperoxide formation by an α-ketoglutarate-dependent mononuclear non-haem iron enzyme.撤稿说明:由α-酮戊二酸依赖性单核非血红素铁酶形成内过氧化物。
Nature. 2021 May;593(7860):612. doi: 10.1038/s41586-021-03527-x.
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An Iron(IV)-Oxo Intermediate Initiating l-Arginine Oxidation but Not Ethylene Production by the 2-Oxoglutarate-Dependent Oxygenase, Ethylene-Forming Enzyme.铁(IV)-氧中间体引发 l-精氨酸氧化但不引发 2-氧代戊二酸依赖性加氧酶,乙烯形成酶产生乙烯。
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Pathway from N-Alkylglycine to Alkylisonitrile Catalyzed by Iron(II) and 2-Oxoglutarate-Dependent Oxygenases.铁(II)和 2-氧代戊二酸依赖的加氧酶催化 N-烷基甘氨酸到烷基异腈的途径。
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Hydrogen Donation but not Abstraction by a Tyrosine (Y68) during Endoperoxide Installation by Verruculogen Synthase (FtmOx1).酪氨酸(Y68)在-verruculogen 合酶(FtmOx1)中环内过氧化物安装过程中供氢而不是夺氢。
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