四氢糠醇在 γ-Al2O3 催化剂上脱水成二氢吡喃:利用原位 DRIFT 光谱监测反应

IF 2.8 3区 化学 Q2 CHEMISTRY, APPLIED Topics in Catalysis Pub Date : 2024-07-10 DOI:10.1007/s11244-024-01989-7
J. A. Pulido, F. Vila, D. Martin Alonso, M. López Granados, R. Mariscal
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引用次数: 0

摘要

本研究采用原位漫反射红外傅立叶变换(DRIFT)光谱分析了四氢糠醇(THFA)脱水成 3,4-二氢-2H-吡喃(DHP)过程中的表面反应性。以活化的 γ-Al2O3 为催化剂,在 648 K 的气相条件下进行 THFA 的脱水反应。在这些条件下,固定床反应器中的 DHP 收率为 84%,催化剂在 70 小时后没有失活迹象。DRIFT 原位光谱法获得的信息取决于反应条件,气相中 THFA 的浓度是一个关键变量。此外,还对气流的温度和时间进行了研究。通过这项技术,可以确定相关产品 DHP、反应过程中在催化剂表面形成的带有羰基(C = O)的两种产品,以及表面物质与氧化物催化剂氧原子反应形成的羧酸盐。这一点意义重大,因为了解了反应过程中表面发生的分子过程,就可以合理设计催化剂,增强其催化特性。因此,原位 DRIFT 光谱是研究 THFA 脱水反应中活性催化剂的重要工具。
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Dehydration of Tetrahydrofurfuryl Alcohol Into Dihydropyran on γ-Al2O3 Catalyst: Reaction Monitoring by In Situ DRIFT Spectroscopy

In this study, in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy was used to analyze the surface reactivity during the dehydration of tetrahydrofurfuryl alcohol (THFA) to 3,4-dihydro-2H-pyran (DHP). The dehydration reaction of THFA is carried out in the gas phase at 648 K using activated γ-Al2O3 as catalyst. Under these conditions, a yield of 84% DHP is obtained in a fixed-bed reactor and the catalyst shows no signs of deactivation after 70 h. The information obtained with DRIFT in situ spectroscopy depends on the reaction conditions, with the concentration of THFA in the gas phase being a critical variable. The temperature and time on stream have also been studied. This technique has allowed to identify DHP, the product of interest, two products with carbonyl group (C = O) formed in the surface of the catalyst during the reaction, and also the formation of carboxylates from the reaction of surface species with the oxygens of the oxide catalyst. This is of considerable significance, as an understanding of the molecular processes occurring at the surface during the reaction would permit the rational design of catalysts to enhance their catalytic properties. Therefore, in situ DRIFT spectroscopy is a valuable tool for studying active catalysts in the THFA dehydration reaction.

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来源期刊
Topics in Catalysis
Topics in Catalysis 化学-物理化学
CiteScore
5.70
自引率
5.60%
发文量
197
审稿时长
2 months
期刊介绍: Topics in Catalysis publishes topical collections in all fields of catalysis which are composed only of invited articles from leading authors. The journal documents today’s emerging and critical trends in all branches of catalysis. Each themed issue is organized by renowned Guest Editors in collaboration with the Editors-in-Chief. Proposals for new topics are welcome and should be submitted directly to the Editors-in-Chief. The publication of individual uninvited original research articles can be sent to our sister journal Catalysis Letters. This journal aims for rapid publication of high-impact original research articles in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
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