当前位置: X-MOL 学术J. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Propene oligomerization on Beta zeolites: Development of a microkinetic model and experimental validation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2021-01-21 , DOI: 10.1016/j.jcat.2021.01.018
Sergio Vernuccio , Elizabeth E. Bickel , Rajamani Gounder , Linda J. Broadbelt

The microkinetic modelling methodology that we developed previously to describe Brønsted acid-catalyzed propene oligomerization on medium-pore MFI zeolites has been extended successfully to large-pore Beta zeolites. The extension of the model was supported by the identification of the key descriptors that account for the different topologies and acid strengths of the zeolite frameworks (physisorption enthalpies, stabilization enthalpies, frequency factors). The model is validated with experimental conversion and selectivity data measured in a plug-flow reactor on a commercial Beta zeolite over a range of operating conditions. Analysis of net reaction rates allowed identifying the preferred pathways that increase oligomerization selectivity toward C9 species with increasing propene pressure. The model was additionally used to investigate how the stabilization enthalpies of chemisorbed intermediates, an important catalyst descriptor, influenced the selectivity and surface coverage at iso-conversion. This analysis provides mechanistic insights into the propene oligomerization reaction network and its dependence on zeolite topology, and demonstrates how microkinetic models can describe catalyst behaviour and aid in catalyst and process optimization.



中文翻译:

β沸石上的丙烯低聚:微观动力学模型的开发和实验验证

我们先前开发的用于描述布朗斯台德酸催化的丙烯在中孔MFI沸石上进行寡聚的微观动力学建模方法已成功扩展到大孔Beta沸石。该模型的扩展得到了关键描述符的支持,这些描述符说明了沸石骨架的不同拓扑和酸强度(物理吸附焓,稳定焓,频率因子)。该模型通过在商业化Beta沸石上的活塞流反应器中在一定范围的操作条件下测得的实验转化率和选择性数据进行验证。净反应速率的分析可以确定增加对C 9的低聚选择性的优选途径丙烯压力增加的物种。该模型还用于研究化学吸附的中间体的稳定化焓,一个重要的催化剂描述符,在如何影响选择性和表面覆盖γ变换。该分析提供了对丙烯低聚反应网络及其对沸石拓扑结构的依赖性的机械见解,并展示了微动力学模型如何描述催化剂行为并有助于催化剂和工艺优化。

更新日期:2021-02-16
down
wechat
bug