Coupling Alkane Dehydrogenation with Hydrogenation Reactions on Cation-Exchanged Zeolites

该项目的目标是扩大以前的努力，利用烷烃作为氢气来源，直接与硫磺反应来脱除碳氢化合物。使用氢气进行脱硫需要昂贵且耗能的蒸汽重整或天然气的部分氧化。如果富含氢气的烷烃可以在加工过程中直接用于脱除硫化氢中的硫，那么它们就可以提供替代氢源。在以前的工作中，这一概念的可行性是通过丙烷-噻吩混合物在锌和钴交换沸石上的反应来论证的。目前的工作将这种化学扩展到更广泛的阳离子交换沸石，包括甲烷和高级烃在内的氢源，以及更难处理的硫和氮化合物。此外，还将研究耦合加氢-脱氢要求的机理以及阳离子和酸中心在化学中的具体作用，目的是开发预测结构-功能规则，以指导更有效的催化剂的合成。这种脱除硫的技术可能为高效和环境友好的工艺奠定基础。

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.