Reactivity and Structure of Complex Sulfides in the Oxidative Methane Coupling with Soft Oxidants

由于自然保护区中甲烷资源丰富，且以乙烯为原料的价值较高，甲烷直接氧化偶联制取乙烯具有很高的经济价值。首先，关于使用硫磺气体作为氧化剂的研究结果很有希望，但到目前为止，对相对狭窄的材料范围内的研究还很少。本研究的主要目的是系统地探索甲烷与硫磺气体等软氧化剂氧化偶联反应中不同类型的硫化物，以期筛选出对该反应最具活性和选择性的催化剂。此外，还建议进行将还原气体混合到反应物进料中的测量。这可以防止过氧化生成二硫化碳。通过将反应器测量与显微和光谱研究相结合，可以找到关于催化活性相的信息，并可以确定有利于或不利于甲烷高转化率为乙烯的催化剂特性。

Due to the abundance of methane in natural reserves and the high value of ethylene as raw material, the direct oxidative coupling of methane to ethylene is of high economical interest. First results on the use of sulfur gas as oxidant are promising but only few studies on a relatively narrow range of materials have been performed so far.The major aim of this study is to systematically explore different types of sulfides in the oxidative coupling of methane with soft oxidants such as sulfur gas in order to down-select the most active and selective catalysts for this reaction. Furthermore, it is proposed to perform measurements in which a reducing gas is mixed to the reactant feed. This could prevent the overoxidation to carbon disulfide. By combining the reactor measurements with microscopic and spectroscopic investigations, information on the catalytically active phase may be found and catalyst features which favor or disfavor a high conversion of methane to ethylene could be identified.