Overcoming limitations in propanedehydrogenation by codesigning catalyst-membrane systems

• 成果类型: Article
• 署名作者: Almallahi, Rawan; Wortman, James; Linic, Suljo
• 署名单位: University of Michigan System; University of Michigan; University of Michigan System; University of Michigan
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8370
• DOI: 10.1126/science.adh3712
• 发表日期: 2024-03-22
• 页码: 1325-1331
• 关键词: pt-sn catalysts; propane dehydrogenation; gallium oxide; oxidative dehydrogenation; light alkanes; reactor; performance; deactivation; selectivity; reduction

摘要

Propylene production through propane dehydrogenation (PDH) is endothermic, and high temperatures required to achieve acceptable propane conversions lead to low selectivity and severe carbon-induced deactivation of conventional catalysts. We developed a catalyst-membrane system that removes the hydrogen by-product and can thus achieve propane conversions that exceed equilibrium limits. In this codesigned system, a silica/alumina (SiO2/Al2O3) hollow-fiber hydrogen membrane was packed with a selective platinum-tin (Pt1Sn1/SiO2) PDH catalyst on the tube side with hydrogen diffusing from the tube to the shell side. We demonstrate that the catalyst-membrane system can achieve propane conversions >140% of the nominal equilibrium conversion with a propylene selectivity >98% without deactivation of the system components. We also show that by introducing oxygen on the shell side of the catalyst-membrane system, we can couple the endothermic PDH reaction on the tube side with exothermic hydrogen oxidation on the shell side. This coupling results in higher rates of hydrogen transport, leading to further enhancements in the propane conversion as well as desired thermoneutral system operation.