分级H-ZSM-5介孔结构对正丁醇脱水的影响

IF 5.1 Q2 ENGINEERING, CHEMICAL
Phebe Lemaire, Arno de Reviere, Dhanjay Sharma, Valérie Ruaux, Jaouad Al Atrach, Valentin Valtchev, Joris Thybaut, Maarten Sabbe and An Verberckmoes*, 
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引用次数: 0

摘要

沸石是石油化学工业中应用最广泛的催化剂之一。然而,由于其复杂的微孔网络,它们容易受到扩散限制和失活。为了克服这些限制,已经提出了几种修改方法,每种方法都显示出其优点。在这项工作中,两种最有前途的策略被结合在一起,即在合成过程中限制晶体轴的长度以实现片状形态,并引入介孔,创建分层片状H-ZSM-5。在合成混合物中加入尿素作为生长调节剂获得了片状形貌,并通过NaOH/TPAOH混合物蚀刻在片状H-ZSM-5中引入介孔。作为基准,同样的蚀刻过程应用于商业ZSM-5对应物。在正丁醇脱水实验中,这些材料的片状形态表现出更好的催化性能,显著提高了每个酸位的活性和稳定性,并略微提高了对丁烯的选择性。商业ZSM-5中介孔的产生也增加了每个酸位的活性,但降低了催化剂的稳定性,可能是由于蚀刻时刘易斯酸位的数量增加。将相同的改性方法应用于类板H-ZSM-5时,观察到更大的介孔和一些大孔。这些进一步增加了催化剂的稳定性,但几乎没有影响每个酸位点的活性,可能是由于已经优化的板状H-ZSM-5的催化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The Influence of Mesopore Architecture in Hierarchical H-ZSM-5 on n-Butanol Dehydration

Zeolites are among the most widely employed catalysts in the (petro-)chemical industry. However, due to their elaborate microporous network, they are prone to diffusion limitations and deactivation. Several modification methods have been proposed to overcome these limitations, each exhibiting their benefits. In this work, two of the most promising strategies were combined, i.e., limiting the length of one of the crystal axes during synthesis to achieve a platelike morphology and introducing mesoporosity, creating a hierarchical platelike H-ZSM-5. The platelike morphology was obtained by adding urea as a growth modifier to the synthesis mixture, and mesopores were introduced in the platelike H-ZSM-5 through etching with a NaOH/TPAOH mixture. As a benchmark, the same etching procedure was applied to a commercial ZSM-5 counterpart. These materials were tested in the n-butanol dehydration, where the platelike morphology exhibited an improved catalytic performance, significantly increasing the activity per acid site and stability, and slightly increasing the selectivity toward the butenes. The generation of mesopores in commercial ZSM-5 also increased the activity per acid site but reduced the catalyst’s stability, likely due to an increased amount of Lewis acid sites upon etching. When applying the same modification method to the platelike H-ZSM-5, much larger mesopores and some macropores were observed. These further increased the stability of the catalyst but barely affected the activity per acid site, presumably due to the already optimized catalytic performance of the platelike H-ZSM-5.

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来源期刊
ACS Engineering Au
ACS Engineering Au 化学工程技术-
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期刊介绍: )ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)
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