Gołąbek Kinga, Tarach Karolina A, Filek Urszula, Góra-Marek Kinga
Faculty of Chemistry, Jagiellonian University in Kraków, 2 Gronostajowa St., 30-387 Kraków, Poland.
Jerzy Haber Institute of Catalysis and Surface Chemistry PAS, Niezapominajek 8, Kraków, Poland.
Spectrochim Acta A Mol Biomol Spectrosc. 2018 Mar 5;192:464-472. doi: 10.1016/j.saa.2017.11.049. Epub 2017 Nov 23.
In this work, the role of pore arrangement of 10-ring zeolites ZSM-5, TNU-9 and IM-5 on their catalytic properties in ethanol transformation were investigated. Among all the studied catalysts, the zeolite IM-5, characterized by limited 3-dimensionality, presented the highest conversion of ethanol and the highest yields of diethyl ether (DEE) and ethylene. The least active and selective to ethylene and C products was zeolite TNU-9 with the largest cavities formed on the intersection of 10-ring channels. The catalysts varied, however, in lifetime, and their deactivation followed the order: IM-5>TNU-9>ZSM-5. The processes taking place in the microporous zeolite environment were tracked by IR spectroscopy and analysed by the 2D correlation analysis (2D COS) allowing for an insight into the nature of chemisorbed adducts and transition products of the reaction. The cage dimension was found as a decisive factor influencing the tendency for coke deposition, herein identified as polymethylated benzenes, mainly 1,2,4-trimethyl-benzene.
在本工作中,研究了10元环沸石ZSM - 5、TNU - 9和IM - 5的孔道排列对其乙醇转化催化性能的影响。在所有研究的催化剂中,具有有限三维结构的IM - 5沸石表现出最高的乙醇转化率以及最高的二乙醚(DEE)和乙烯产率。对乙烯和C产物活性和选择性最低的是TNU - 9沸石,它在10元环通道交叉处形成了最大的孔穴。然而,催化剂的寿命有所不同,其失活顺序为:IM - 5>TNU - 9>ZSM - 5。通过红外光谱跟踪在微孔沸石环境中发生的过程,并通过二维相关分析(2D COS)进行分析,从而深入了解反应中化学吸附加合物和过渡产物的性质。发现笼尺寸是影响焦炭沉积倾向的决定性因素,在此处焦炭主要被鉴定为多甲基化苯,尤其是1,2,4 - 三甲基苯。