Deactivation of NaY in Aniline Alkylation with Methanol: Accumulation Kinetics, Composition, and Localization of Coke Deposits

IF 1.1 4区工程技术 Q3 CHEMISTRY, ORGANIC

Petroleum Chemistry Pub Date : 2025-07-23 DOI:10.1134/S0965544125600912

V. S. Pavlov, O. A. Ponomareva, D. V. Bruter, I. V. Dobryakova, I. A. Kostyukov, O. I. Grinevich, A. K. Buryak, V. L. Zholobenko, I. I. Ivanova

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Abstract

This study investigates the kinetics of deactivation of a commercial NaY zeolite catalyst in alkylation of aniline with methanol due to coke deposition. In order to identify the accumulation trend, composition, and localization of coke deposits, a series of zeolite catalyst samples differing in reactor residence time were obtained. The catalysts and the accumulated coke deposits were characterized by X-ray fluorescence analysis, X-ray powder diffraction, TGA/DTA, SEM, low-temperature nitrogen adsorption, ²⁷Al and ¹³C MAS NMR, NH₃-TPD, and GC/MS. The coke species deposited on the catalyst during the reaction were found to mostly consist of long-chain aliphatic compounds (mainly alkanes) and heterocyclic aromatics. Both the TGA and GC/MS data showed that the relative content of aliphatic compounds increased with the progress of the catalyst deactivation. Moreover, the variation in the zeolite’s interplanar distances (measured by XRD) showed that the aliphatics were mainly localized in the zeolite pores.

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苯胺与甲醇烷基化过程中NaY失活：积累动力学、组成和焦炭沉积物的局部化

本文研究了苯胺与甲醇烷基化反应中焦炭沉积引起的NaY沸石催化剂失活动力学。为了确定焦炭沉积物的富集趋势、组成和位置，获得了一系列不同反应器停留时间的沸石催化剂样品。采用x射线荧光分析、x射线粉末衍射、TGA/DTA、SEM、低温氮吸附、27Al和13C MAS NMR、NH3-TPD和GC/MS对催化剂和积炭进行了表征。在反应过程中，沉积在催化剂上的焦炭主要由长链脂肪族化合物（主要是烷烃）和杂环芳烃组成。TGA和GC/MS数据均表明，随着催化剂失活的进行，脂肪族化合物的相对含量逐渐增加。此外，分子筛的面间距变化（XRD测量）表明，脂肪族主要集中在沸石孔隙中。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Petroleum Chemistry 工程技术-工程：化工

CiteScore

2.50

自引率

21.40%

发文量

102

审稿时长

6-12 weeks

期刊介绍： Petroleum Chemistry (Neftekhimiya), founded in 1961, offers original papers on and reviews of theoretical and experimental studies concerned with current problems of petroleum chemistry and processing such as chemical composition of crude oils and natural gas liquids; petroleum refining (cracking, hydrocracking, and catalytic reforming); catalysts for petrochemical processes (hydrogenation, isomerization, oxidation, hydroformylation, etc.); activation and catalytic transformation of hydrocarbons and other components of petroleum, natural gas, and other complex organic mixtures; new petrochemicals including lubricants and additives; environmental problems; and information on scientific meetings relevant to these areas. Petroleum Chemistry publishes articles on these topics from members of the scientific community of the former Soviet Union.