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Mechanistic aspects of n-paraffins hydrocracking: Influence of zeolite morphology and acidity of Pd(Pt)/ZSM-5 catalysts
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-07-06 , DOI: 10.1016/j.jcat.2020.06.031
Lingqian Meng , Gina Vanbutsele , Robert Pestman , Andreas Godin , Douglas E. Romero , Arno J.F. van Hoof , Lu Gao , Tobias F. Kimpel , Jiachun Chai , Johan A. Martens , Emiel J.M. Hensen

The influence of zeolite domain size, acidity, and metal type on n-decane and n-nonadecane hydroconversion was investigated for bifunctional Pd(Pt)/ZSM-5 zeolite (bulk, desilicated, thin and thick nanosheets). Decreasing the size of zeolitic domains to a few nanometers results in lower overall activity, higher skeletal isomerization yield, and an imbalance between metal and acid functions. These changes are attributed to a lower pore occupancy of olefinic intermediates due to the substantially larger external surface of nanosheets and higher desorption rates. Well-balanced bifunctional behavior and higher activity of nanosheet ZSM-5 can be achieved by strengthening the metal function or lowering the acidity. The influence on the isomerized and cracked product fractions is also discussed. Hydroconversion of n-nonadecane gave low yields of skeletal isomers over all Pd-loaded ZSM-5 catalysts and led to significant over-cracking due to the long intracrystalline residence times of the long hydrocarbon reactant.



中文翻译:

构烷烃加氢裂化的机理方面:沸石形态和Pd(Pt)/ ZSM-5催化剂酸度的影响

沸石畴尺寸,酸度和金属类型对癸烷和癸烷的影响研究了双官能Pd(Pt)/ ZSM-5沸石(散装,脱硅酸盐,薄和厚纳米片)的十八烷加氢转化。将沸石结构域的尺寸减小到几纳米会导致较低的总体活性,较高的骨架异构化产率以及金属和酸功能之间的不平衡。这些变化归因于烯烃中间产物的较低的孔占有率,这归因于纳米片的外表面明显更大和较高的解吸速率。通过增强金属功能或降低酸度,可以实现纳米片ZSM-5平衡的双功能行为和更高的活性。还讨论了对异构化和裂解产物级分的影响。n-的加氢转化在所有负载钯的ZSM-5催化剂上,十八碳烯的骨架异构体的收率均较低,并且由于长烃反应物的晶内停留时间较长,导致严重的超裂。

更新日期:2020-07-18
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