Promoting role of residual organic structure directing agent in skeletal butene isomerization over ferrierite

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Karoline L. Hebisch, Pawel A. Chmielniak, Violet A. Cutler, Rick B. Watson, Kinga Gołąbek, Carsten Sievers
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Abstract

This work examines how acid site concentration (FT-IR) and strength (NH3-TPD) as well as pore mouth accessibility modulate the activity of the microporous zeolite ferrierite (H-FER) during the skeletal isomerization of 1-butene to iso-butene. Restricting the accessibility of catalyst pores and strong acid sites is achieved by selective oxidation of residual organic structure directing agent (OSDA) through precise control of calcination conditions. Because this reaction is mediated by catalytically active carbonaceous deposits, residual OSDA affects their formation. This work demonstrates that small amounts of residual OSDA (∼ 0.2 wt%) are beneficial to the reaction under industrially relevant reaction conditions in three ways. Selective poisoning of strong BAS with OSDA nearly halves the amount of dimerization and cracking byproducts and improves catalyst lifetime. Simultaneously, carbonaceous fragments of the OSDA act as coke precursors and help shorten the startup time. Hence, catalyst lifetime may be significantly improved through both optimal pre-treatment conditions and by designing catalysts with an increased number of accessible pore mouths.

Abstract Image

残余有机结构引导剂在铁氧体上的骨架丁烯异构化中的促进作用
这项研究探讨了在 1-丁烯向异丁烯的骨架异构化过程中,酸位点浓度(傅立叶变换红外光谱)和强度(NH3-TPD)以及孔口可及性如何调节微孔沸石铁氧体(H-FER)的活性。通过精确控制煅烧条件,对残留的有机结构引导剂(OSDA)进行选择性氧化,从而限制催化剂孔隙和强酸位点的可及性。由于该反应是由具有催化活性的碳质沉积物介导的,因此残留的 OSDA 会影响其形成。这项研究表明,在工业相关的反应条件下,少量的残留 OSDA(0.2 wt%)在三个方面有利于反应的进行。用 OSDA 对强 BAS 进行选择性毒化可将二聚化和裂解副产物的数量减少近一半,并延长催化剂的使用寿命。同时,OSDA 的碳质碎片可作为焦炭前体,有助于缩短启动时间。因此,通过优化预处理条件和设计具有更多可进入孔口的催化剂,可以显著提高催化剂的使用寿命。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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