Study of the Methanol Conversion into Dimethyl Ether Obtained in the Process of Biomimetic Methane Monooxidation by Hydrogen Peroxide

G. Nahmatova, Latifa Gasanova, Tofig Nagiev
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Abstract

The monooxidation of methane into methanol was carried out on biomimetic heterogeneous catalyst – iron pentafluorotetraphenylporphyrin on Al2O3 (ImtOH), at atmospheric pressure and temperatures of 200-350°C, which resulted in liquid one-carbon compounds CH3OH (19.2%), CH2O (1.55%), CH3OCH3 (8.2%) with high selectivity and are widely used in the chemical industry. In order to establish the routes of these products formation and the mechanism for the methane conversion into them, the investigation of the methanol conversion reaction was carried out, as an intermediate compound of the methane oxidation, under identical conditions on the same catalyst.The result was only dimethyl ether with 100% selectivity. This proved that in this reaction system, methanol obtained from the methane monooxidation is converted only into dimethyl ether, and formaldehyde, in parallel with methanol, is formed from methane. The mechanisms of the elementary stages of the formation of methanol, formaldehyde and dimethyl ether on the surface of the bioimitator through the formation of an active complex (ImtOOH) are presented, in which the unity of the mechanisms of redox and acid-base catalysis traced within the framework of the principle of the bond redistribution chain (BRC), similar to enzymatic reactions.
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过氧化氢模拟甲烷单氧化过程中甲醇转化为二甲醚的研究
在常压和 200-350°C 温度条件下,在仿生物异相催化剂 - Al2O3(ImtOH)上的五氟四苯基卟啉铁上进行了甲烷转化为甲醇的单氧化反应,生成了高选择性的液态一碳化合物 CH3OH(19.2%)、CH2O(1.55%)、CH3OCH3(8.2%),广泛应用于化学工业。为了确定这些产物的形成途径以及甲烷转化为这些产物的机理,在相同的催化剂上,在相同的条件下,对甲烷氧化的中间化合物甲醇转化反应进行了研究。这证明了在该反应体系中,甲烷一氧化反应生成的甲醇只转化为二甲醚,而甲醛则与甲醇同时从甲烷中生成。文中介绍了通过形成活性复合物(ImtOOH)在生物引发剂表面形成甲醇、甲醛和二甲醚的初级阶段的机理,其中在类似酶促反应的键重新分布链(BRC)原理框架内追踪了氧化还原和酸碱催化机理的统一性。
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