Effects of Cerium Oxide Incorporation and Zeolite Cationic Form on ZSM-5 Catalysts for Glycerol Dehydration

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-09-13 DOI:10.1007/s10562-025-05169-4

Billy Joy Vargas, Caroline Pereira Roldão, Rui dos Santos Ferreira Filho, Juliana Oliveira Fernandes, Edilene Deise da Silva Ferracine, Cezar Augusto da Rosa, Vanessa Bongalhardo Mortola

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Abstract

NaZSM-5, HZSM-5, and Ce/HZSM-5 zeolites with a Si/Al ratio of 25 were synthesized via a hydrothermal method developed by our research group, which enables the formation of hierarchical ZSM-5 structures with micro and mesoporosity. These materials were evaluated as catalysts for the glycerol dehydration reaction. The incorporation of cerium oxide into HZSM-5 introduced redox properties that enhanced catalyst stability under oxygen-deficient conditions. When air was co-fed, the oxidative removal of carbonaceous deposits promoted sustained catalytic activity, with Ce/HZSM-5 maintaining consistent performance under both oxidizing and non-oxidizing environments. HZSM-5 also demonstrated stable activity in the presence of oxygen, benefiting from surface regeneration. In contrast, NaZSM-5 exhibited the lowest selectivity, producing a broader range of by-products, a behavior attributed to its lower surface area, limited mesoporosity, and reduced concentration of strong acid sites. These findings highlight the critical role of hierarchical structure, acidity, and redox functionality in enhancing the activity and selectivity of zeolite-based catalysts for acrolein production.

Graphical Abstract

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氧化铈掺入和沸石阳离子形态对ZSM-5催化剂甘油脱水性能的影响

本课课组采用水热法合成了Si/Al比为25的ZSM-5、HZSM-5和Ce/HZSM-5分子筛，形成了具有微孔和介孔的分级结构。对这些材料作为甘油脱水反应的催化剂进行了评价。在HZSM-5中掺入氧化铈可以引入氧化还原特性，增强催化剂在缺氧条件下的稳定性。当空气共进时，氧化去除碳质沉积物促进了持续的催化活性，Ce/HZSM-5在氧化和非氧化环境下都保持一致的性能。HZSM-5在氧气存在下也表现出稳定的活性，有利于表面再生。相比之下，NaZSM-5表现出最低的选择性，产生更广泛的副产物，这一行为归因于其较低的表面积、有限的介孔和较低的强酸位点浓度。这些发现强调了层次结构、酸度和氧化还原功能在提高沸石基催化剂生产丙烯醛的活性和选择性方面的关键作用。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.