Marinkovic Jakob Maximilian, Benders Stefan, Garcia-Suarez Eduardo J, Weiß Alexander, Gundlach Carsten, Haumann Marco, Küppers Markus, Blümich Bernhard, Fehrmann Rasmus, Riisager Anders
Technical University of Denmark, Centre for Catalysis and Sustainable Chemistry, Department of Chemistry Kemitorvet, Building 207, 2800 Kgs. Lyngby Denmark
RWTH Aachen University, Institut für Technische und Makromolekulare Chemie Worringerweg 2 52064 Aachen Germany.
RSC Adv. 2020 May 15;10(31):18487-18495. doi: 10.1039/c9ra09515b. eCollection 2020 May 10.
Monolithic silicon carbide supported ionic liquid-phase (SILP) Rh-catalysts have very recently been introduced for gas-phase hydroformylation as an important step toward industrial upscaling. This study investigates the monolithic catalyst system in combination with different impregnation procedures with non-invasive magnetic resonance imaging (MRI). The findings were supported by X-ray microtomography (micro-CT) data of the monolithic pore structure and a catalytic performance test of the catalyst system for 1-butene gas-phase hydroformylation. MRI confirmed a homogeneous impregnation of the liquid phase throughout the full cross-section of the cylindrical monoliths. Consistent impregnations from one side to the other of the monoliths were achieved with a stabilizer in the system that helped preventing inhomogeneous rim formation. External influences relevant for industrial application, such as long-term storage and temperature exposure, did not affect the homogeneous liquid-phase distribution of the catalyst. The work elucidates important parameters to improve liquid-phase catalyst impregnation to obtain efficient monolithic catalysts for industrial exploitation in gas-phase hydroformylation as well as other important industrial processes.
整体式碳化硅负载离子液体相(SILP)铑催化剂最近被引入用于气相氢甲酰化反应,这是迈向工业规模扩大的重要一步。本研究结合不同的浸渍程序,利用非侵入式磁共振成像(MRI)对整体式催化剂体系进行了研究。整体式孔结构的X射线显微断层扫描(micro-CT)数据以及该催化剂体系用于1-丁烯气相氢甲酰化反应的催化性能测试结果支持了这些发现。MRI证实液相在圆柱形整体式载体的整个横截面上均匀浸渍。通过在体系中加入稳定剂,实现了从整体式载体一侧到另一侧的均匀浸渍,有助于防止形成不均匀的边缘。与工业应用相关的外部影响,如长期储存和温度暴露,并未影响催化剂的均匀液相分布。这项工作阐明了改善液相催化剂浸渍的重要参数,以获得用于气相氢甲酰化反应以及其他重要工业过程的高效整体式催化剂,用于工业开发。