Myoglobin Reconstituted with Ni Tetradehydrocorrin as a Methane‐Generating Model of Methyl‐coenzyme M Reductase
Myoglobin Reconstituted with Ni Tetradehydrocorrin as a Methane‐Generating Model of Methyl‐coenzyme M Reductase
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用 Ni 四氢可林重构肌红蛋白作为甲基辅酶 M 还原酶的甲烷生成模型
DOI：
10.1002/anie.201907584
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Hayashi Takashi
中科院分区：
文献类型：
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作者：
Oohora Koji;Miyazaki Yuta;Hayashi Takashi
用 Ni 四氢可林重组肌红蛋白作为含 F430 的甲基辅酶 M 还原酶的模型进行了研究，该还原酶催化厌氧甲烷的产生。 NiII四氢咕啉配合物的NiII/NiI氧化还原电位相对于SHE为-0.34 V，EPR光谱表明在连二亚硫酸盐还原时形成了NiI物质。该氧化还原电位比 F430 的氧化还原电位高约 0.31 V。 NiTetrade Hydrocorrin 部分与肌红蛋白的脱辅基形式结合，产生重组蛋白。在还原条件下，在重构蛋白存在的情况下，模型与碘甲烷反应会产生甲烷气体，而 NiI 复合物本身不会产生甲烷气体。这是基于蛋白质的含 F430 甲基辅酶 M 还原酶功能模型的第一个例子。
Myoglobin reconstituted with Ni tetradehydrocorrin was investigated as a model of F430‐containing methyl‐coenzyme M reductase, which catalyzes anaerobic methane generation. The NiIItetradehydrocorrin complex has a NiII/NiIredox potential of −0.34 V vs. SHE and EPR spectroscopy indicates the formation of a NiIspecies upon reduction by dithionite. This redox potential is approximately 0.31 V more positive than that of F430. The NiItetradehydrocorrin moiety is bound to the apo‐form of myoglobin to yield the reconstituted protein. Methane gas is generated in the reaction of the model with methyl iodide in the presence of the reconstituted protein under reductive conditions, whereas the NiIcomplex itself does not produce methane gas. This is the first example of a protein‐based functional model of F430‐containing methyl‐coenzyme M reductase.