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首页> 外文期刊>Catalysis science & technology >Selective mild oxidation of methane to methanol or formic acid on Fe-MOR catalysts
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Selective mild oxidation of methane to methanol or formic acid on Fe-MOR catalysts

机译：选择温和的甲烷氧化甲醇或甲酸Fe-MOR催化剂

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Controllable methane oxidation directly into value-added products under mild conditions remains a challenge. Herein, an active Fe/MOR catalyst was synthesized via simple solid-state ion exchange, and its activity in the selective oxidation of methane with H2O2 in the aqueous phase was intensively investigated. The octahedral dimeric Fe3+ species [Fe-2(mu-O)(2)] in the extra framework was confirmed as the initial active site by X-ray photoelectron spectroscopy, X-ray absorption near-edge structure and extended X-ray absorption fine structure, UV-vis diffuse-reflectance spectroscopy, and high-angle annular dark-field scanning transmission electron microscopy in combination with DFT calculations. The DFT calculations indicated that methanol formation via methyl peroxide (CH3OOH*) on [Fe-2(mu-OH)(2)O-2] is the most favorable pathway compared to the direct formation of methanol via CH3O*. The formed CH3OH is easily further oxidized by hydroxyl radicals (OH) resulting in non-selective methane oxidation. In contrast, the Fe/MOR catalyst could lead to a high methanol selectivity of 71.3% in the presence of homogeneous Cu2+ precursor, which efficiently suppressed the over-oxidation of methanol, and a high formic acid selectivity up to 81-82% at a slightly higher reaction temperature by mildly shifting the oxidation of methanol and formaldehyde to the target product.
机译：可控甲烷直接氧化成在温和条件下增值产品仍然是一个挑战。通过简单的固体催化剂合成选择性离子交换,它的活动甲烷氧化与过氧化氢溶液阶段是深入调查。八面体二聚的Fe3 +物种[Fe-2 (mu-O) (2)]在被确诊为额外的框架初始活性部位的x射线光电子光谱、x射线吸收靠近边缘和扩展x射线吸收精细结构结构、紫外可见漫反射率环形暗场光谱学,扫描透射电子显微镜结合DFT计算。计算结果表明,甲醇的形成通过过氧化甲基(CH3OOH *)[Fe-2 (mu-OH)(2) 0 2)是最有利的途径相比直接甲醇通过的形成CH3O *。通过羟基自由基(OH)导致氧化无选择性的甲烷氧化。Fe /铁道部可能导致高甲醇催化剂的选择性71.3%齐次Cu2 +前体,有效率抑制的over-oxidation甲醇,甲酸的选择性高达到81 - 82%更高的反应温度温和甲醇的氧化和转移甲醛对目标产品。

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