Catalytic Oxidation of Methane by Wild-Type Cytochrome P450BM3 with Chemically Evolved Decoy Molecules
Catalytic Oxidation of Methane by Wild-Type Cytochrome P450BM3 with Chemically Evolved Decoy Molecules
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DOI：
10.1021/acscatal.3c01158
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发表时间：
2023-06-14
期刊：
影响因子：
12.9
通讯作者：
Shoji, Osami
中科院分区：
文献类型：
--
作者：
Ariyasu, Shinya;Yonemura, Kai;Shoji, Osami
生物甲烷氧化是一种非常理想的将天然气转化为液体的方法，以满足日益增长的燃料和化工原料需求，并减少甲烷排放的温室效应。由于天然血红素酶催化甲烷氧化转化为甲醇的研究尚未发现，因此，包括细胞色素P450（P450s）在内的血红素酶一直被认为不能催化甲烷氧化转化。在10 MPa的高压甲烷下，化学演化的假衬底（诱饵分子）的存在下。我们的研究表明，在室温下甲烷催化转化为甲醇，总转化数为4。
Biological methane oxidation is a highly desirable methodfor theconversion of natural gas into a liquid to meet the increasing demandfor fuel and chemical feedstock as well as reducing the potent greenhouseeffects of methane emissions. Because natural hemoenzymes that cancatalyze the conversion of methane to methanol have not been found,it has long been considered that hemoenzymes, including cytochromeP450s (P450s), cannot catalyze the oxidative conversion of methane.Herein, we report the catalytic oxidation of methane by wild-typeP450BM3, without any mutagenesis, in the presence of chemically evolveddummy substrates (decoy molecules) under high-pressure methane at10 MPa. Our studies showed that methane was catalytically convertedinto methanol at room temperature with a total turnover number of4.