Festa Giovanni, Serrano-Lotina Ana, Meloni Eugenio, Portela Raquel, Ruocco Concetta, Martino Marco, Palma Vincenzo
Department of Industrial Engineering, University of Salerno, Via Giovanni Paolo II 132, 84084 Fisciano, Salerno, Italy.
Instituto de Catalisis y Petroleoquimica (ICP), CSIC, C/ Marie Curie 2. 28049 Madrid, Spain.
Ind Eng Chem Res. 2024 Sep 12;63(38):16269-16284. doi: 10.1021/acs.iecr.3c04089. eCollection 2024 Sep 25.
Propane dehydrogenation reaction (PDH) is an extremely attractive way to produce propylene; however, the catalysts often lead to byproduct formation and suffer from deactivation. This research focuses on the development of efficient Pt/Sn-based shaped catalysts by utilizing Mg-modified mesoporous silica, sepiolite (natural SiMgO mesoporous clay), and sepiolite/bentonite/alumina as supports with the aim of achieving superior stability and selectivity for industrial propylene production by PDH. The catalysts were prepared by sequential impregnation of the supports with the corresponding solutions of tin chloride and platinum chloride, by obtaining a nominal loading of 0.7 wt % of Sn and 0.5 wt % of Pt. A range of analytical techniques were used to characterize the catalysts, including X-ray diffraction, nitrogen physisorption isotherms, Hg intrusion porosimetry, thermogravimetric analyses, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. The basicity of the catalysts was assessed using carbon dioxide temperature-programmed desorption (CO-TPD). The results confirm that the support material plays a critical role in catalyst performance; in particular, the presence of weak basic sites, due to magnesium addition, improved selectivity to propylene and reduced coke formation. Catalytic pellets of Sn-Pt supported on macroporous sepiolite or sepiolite and bentonite-modified mesoporous alumina performed comparably with propane conversion very close to thermodynamic equilibrium and selectivity to propylene above 95%. The latter support led to improved stability and was regenerated at milder temperatures, making it suitable for industrial applications.
丙烷脱氢反应(PDH)是一种极具吸引力的生产丙烯的方法;然而,催化剂常常会导致副产物的形成且容易失活。本研究聚焦于通过利用镁改性的介孔二氧化硅、海泡石(天然SiMgO介孔粘土)以及海泡石/膨润土/氧化铝作为载体来开发高效的Pt/Sn基成型催化剂,旨在通过PDH实现工业生产丙烯时具有卓越的稳定性和选择性。通过用氯化锡和氯化铂的相应溶液依次浸渍载体来制备催化剂,锡的标称负载量为0.7 wt%,铂的标称负载量为0.5 wt%。使用了一系列分析技术对催化剂进行表征,包括X射线衍射、氮物理吸附等温线、压汞法、热重分析、透射电子显微镜、拉曼光谱以及X射线光电子能谱。使用二氧化碳程序升温脱附(CO-TPD)来评估催化剂的碱性。结果证实载体材料在催化剂性能中起着关键作用;特别是,由于添加了镁而存在的弱碱性位点提高了对丙烯的选择性并减少了焦炭的形成。负载在大孔海泡石或海泡石以及膨润土改性的介孔氧化铝上的Sn-Pt催化颗粒在丙烷转化率非常接近热力学平衡且对丙烯的选择性高于95%方面表现相当。后一种载体提高了稳定性并且在较温和的温度下可再生,使其适用于工业应用。