Cindy-Ly Tavera-Méndez , Jose Alirio Mendoza Mesa , Carlos-Alexander Trujillo , Julio César Vargas
{"title":"商用沸石和中间结构 Y 沸石的烷基芳香族质量迁移-酸度特性与裂解反应催化行为的相关性","authors":"Cindy-Ly Tavera-Méndez , Jose Alirio Mendoza Mesa , Carlos-Alexander Trujillo , Julio César Vargas","doi":"10.1016/j.catcom.2024.106890","DOIUrl":null,"url":null,"abstract":"<div><p>A strategy to mitigate diffusion restrictions associated with heavy crude oil conversions is using mesostructured Y zeolite. In recent years, multiple routes have been proposed for obtaining materials with improved catalytic performance versus catalysts with higher molecular transport restrictions. Typically, after the implementation of these treatments, improvement in catalytic activity is correlated either with changes in textural properties (area and porous volume) or the modification of physicochemical properties (Si/Al ratio and acid strength); however, the correlation with diffusional mass transport characteristics is not typical. In this study, alkylaromatic molecules of different kinetic diameters, such as benzene, toluene, p–xylene, and m–xylene, were used as molecule probes to determine the effective diffusion through a pulse experiment under conditions of no adsorption or reaction. The studied solids include five commercial zeolites from the Zeolyst CBV series and four top–down mesostructured Y zeolites. The obtained concentration curves were fitted to an exponential decay model, a solution of the second Fick's law under defined experimental conditions, and correlation values between 0.9996 > R<sup>2</sup> > 0.9896 were found. Furthermore, the implementation of the descriptors “Transport ratio (TR<sub>MR</sub>)” and “Corrected transport ratio (TR<sub>MR</sub><sup>c</sup>)” was proposed, which allowed the combined representation of the change in the mass transport of aromatic probes and the changes in the acidity of the zeolite, after the application of top–down treatments. These descriptors proved simple and effective tools to correlate the changes after mesopore insertion with the catalytic performance in the 1,3,5–Triisopropylbenzene (TIPB) cracking reaction. Our approach is an integral method of screening mesostructured zeolites with an adequate balance of acidity and transport properties.</p></div>","PeriodicalId":263,"journal":{"name":"Catalysis Communications","volume":"187 ","pages":"Article 106890"},"PeriodicalIF":3.4000,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1566736724000505/pdfft?md5=b55685ad179631c79999bd79f22c2c3c&pid=1-s2.0-S1566736724000505-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Alkylaromatic mass transport – acidity properties correlation for commercial and mesostructured Y zeolites with the catalytic behavior of cracking reactions\",\"authors\":\"Cindy-Ly Tavera-Méndez , Jose Alirio Mendoza Mesa , Carlos-Alexander Trujillo , Julio César Vargas\",\"doi\":\"10.1016/j.catcom.2024.106890\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A strategy to mitigate diffusion restrictions associated with heavy crude oil conversions is using mesostructured Y zeolite. In recent years, multiple routes have been proposed for obtaining materials with improved catalytic performance versus catalysts with higher molecular transport restrictions. Typically, after the implementation of these treatments, improvement in catalytic activity is correlated either with changes in textural properties (area and porous volume) or the modification of physicochemical properties (Si/Al ratio and acid strength); however, the correlation with diffusional mass transport characteristics is not typical. In this study, alkylaromatic molecules of different kinetic diameters, such as benzene, toluene, p–xylene, and m–xylene, were used as molecule probes to determine the effective diffusion through a pulse experiment under conditions of no adsorption or reaction. The studied solids include five commercial zeolites from the Zeolyst CBV series and four top–down mesostructured Y zeolites. The obtained concentration curves were fitted to an exponential decay model, a solution of the second Fick's law under defined experimental conditions, and correlation values between 0.9996 > R<sup>2</sup> > 0.9896 were found. Furthermore, the implementation of the descriptors “Transport ratio (TR<sub>MR</sub>)” and “Corrected transport ratio (TR<sub>MR</sub><sup>c</sup>)” was proposed, which allowed the combined representation of the change in the mass transport of aromatic probes and the changes in the acidity of the zeolite, after the application of top–down treatments. These descriptors proved simple and effective tools to correlate the changes after mesopore insertion with the catalytic performance in the 1,3,5–Triisopropylbenzene (TIPB) cracking reaction. 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引用次数: 0
摘要
减轻与重质原油转化相关的扩散限制的一种策略是使用介质结构 Y 沸石。近年来,人们提出了多种方法来获得催化性能更好的材料与分子传输限制更高的催化剂。通常情况下,在进行这些处理后,催化活性的提高与质构特性(面积和多孔体积)的变化或理化特性(硅/铝比率和酸强度)的改变相关;但与扩散质量迁移特性的相关性并不典型。本研究以苯、甲苯、对二甲苯和间二甲苯等不同动力学直径的烷芳烃分子为分子探针,在无吸附或反应的条件下通过脉冲实验确定有效扩散。所研究的固体包括 Zeolyst CBV 系列的五种商用沸石和四种自上而下的中间结构 Y 沸石。所获得的浓度曲线与指数衰减模型进行了拟合,该模型是第二菲克定律在规定实验条件下的一种解决方案,相关值介于 0.9996 > R > 0.9896 之间。此外,还提出了 "迁移率(TR)"和 "校正迁移率(TR)"描述符,可以综合表示芳香族探针的质量迁移变化和沸石的酸度变化。事实证明,这些描述符是简单有效的工具,可将介孔插入后的变化与 1,3,5-三异丙苯(TIPB)裂解反应的催化性能联系起来。我们的方法是筛选介质结构沸石的一种综合方法,可在酸性和传输特性之间取得适当的平衡。
Alkylaromatic mass transport – acidity properties correlation for commercial and mesostructured Y zeolites with the catalytic behavior of cracking reactions
A strategy to mitigate diffusion restrictions associated with heavy crude oil conversions is using mesostructured Y zeolite. In recent years, multiple routes have been proposed for obtaining materials with improved catalytic performance versus catalysts with higher molecular transport restrictions. Typically, after the implementation of these treatments, improvement in catalytic activity is correlated either with changes in textural properties (area and porous volume) or the modification of physicochemical properties (Si/Al ratio and acid strength); however, the correlation with diffusional mass transport characteristics is not typical. In this study, alkylaromatic molecules of different kinetic diameters, such as benzene, toluene, p–xylene, and m–xylene, were used as molecule probes to determine the effective diffusion through a pulse experiment under conditions of no adsorption or reaction. The studied solids include five commercial zeolites from the Zeolyst CBV series and four top–down mesostructured Y zeolites. The obtained concentration curves were fitted to an exponential decay model, a solution of the second Fick's law under defined experimental conditions, and correlation values between 0.9996 > R2 > 0.9896 were found. Furthermore, the implementation of the descriptors “Transport ratio (TRMR)” and “Corrected transport ratio (TRMRc)” was proposed, which allowed the combined representation of the change in the mass transport of aromatic probes and the changes in the acidity of the zeolite, after the application of top–down treatments. These descriptors proved simple and effective tools to correlate the changes after mesopore insertion with the catalytic performance in the 1,3,5–Triisopropylbenzene (TIPB) cracking reaction. Our approach is an integral method of screening mesostructured zeolites with an adequate balance of acidity and transport properties.
期刊介绍:
Catalysis Communications aims to provide rapid publication of significant, novel, and timely research results homogeneous, heterogeneous, and enzymatic catalysis.