Coupling Alkane Dehydrogenation with Hydrogenation Reactions on Cation-Exchanged Zeolites

该项目的目标是扩展以前的努力，使用烷烃作为氢的来源，直接与硫反应来脱硫碳氢化合物。使用氢气进行脱硫需要昂贵和能源密集型的蒸汽重整或天然气的部分氧化。如果富氢烷烃可以在加工过程中直接使用，以硫化氢的形式去除硫，则可以提供替代的氢源。在以前的工作中，利用丙烷-噻吩混合物在锌和钴交换沸石上的反应证明了这一概念的可行性。目前的工作将这种化学扩展到更广泛的阳离子交换沸石，氢的来源包括甲烷和高级碳氢化合物，以及更难熔的硫和氮化合物。此外，还将研究耦合加氢-脱氢需求的机理以及阳离子和酸位点在化学反应中的特定作用，目的是建立预测结构-功能规则，以指导更有效催化剂的合成。这种脱硫技术可能成为高效和环保工艺的基础。

The objective of the project is to extend previous efforts to desulfurize hydrocarbons using alkanes as a source of hydrogen, with reacts directly with sulfur. The use of hydrogen for desulfurization requires expensive and energy-intensive steam reforming or partial oxidation of natural gas. Hydrogen-rich alkanes offer alternative hydrogen sources if they can be used directly during their processing to remove sulfur as hydrogen sulfide. In previous work the feasibility of this concept was demonstrated using reactions of propane-thiophene mixtures on zinc and cobalt exchanged zeolites. The current work extends this chemistry to a broader range of cation-exchanged zeolites, to sources of hydrogen that include methane and higher hydrocarbons, and to more refractory sulfur and nitrogen compounds. In addition, the mechanism of coupled hydrogenation-dehydrogenation requirements and the specific role of cation and acid sites in the chemistry will be studies with the aim to develop predictive structure-function rules that will guide the synthesis of more effective catalysts. This technique for sulfur removal may form the basis for an efficient and environmentally-benign process.