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Insights into the direct selective oxidation of methane to methanol over ZSM-5 zeolytes in aqueous hydrogen peroxide
Catalysis Today ( IF 5.2 ) Pub Date : 2018-03-22 , DOI: 10.1016/j.cattod.2018.03.031
Saeed Al-Shihri , Christian J. Richard , Hamid Al-Megren , David Chadwick

The direct selective oxidation of methane by aqueous hydrogen peroxide over ZSM-5(50) has been investigated. Methyl hydroperoxide was confirmed as the initial product of methane oxidation. The decomposition of methyl hydroperoxide to formaldehyde is established as a key intermediate in an oxidation pathway to formic acid and ultimately CO2. Hydrogen was detected during the oxidation of methane over ZSM-5 zeolites. The hydrogen was evaluated in terms of its origins and possible role in the production of MeOH. The addition of a copper salt to the ZSM-5(50) zeolite was found to decrease the overall productivity of all methane oxygenates. The use of copper also promoted the selectivity for methyl hydroperoxide whilst removing formic acid. The role of hydroxymethyl-methyl hydroperoxide is considered as an intermediate in the decomposition of methyl hydroperoxide to methanol. A tentative proposal into the nature of the iron species responsible for the catalytic species in ZSM-5(50) is made.



中文翻译:

在过氧化氢水溶液中通过ZSM-5沸石将甲烷直接选择性氧化为甲醇的见解

研究了过氧化氢水溶液在ZSM-5(50)上对甲烷的直接选择性氧化。确认过氧化氢为甲烷氧化的初始产物。氢过氧化物甲基分解为甲醛被确定为通往甲酸和最终CO 2的氧化途径中的关键中间体。在ZSM-5沸石上甲烷氧化过程中检测到氢气。根据氢的来源以及在甲醇生产中的可能作用来评估氢。发现向ZSM-5(50)沸石中添加铜盐会降低所有甲烷含氧化合物的总生产率。铜的使用还促进了氢过氧化甲基的选择性,同时去除了甲酸。羟甲基-甲基氢过氧化物的作用被认为是甲基氢过氧化物分解为甲醇的中间体。提出了关于ZSM-5(50)中负责催化物种的铁物种的性质的初步建议。

更新日期:2018-03-22
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