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基于改进分离方法的不同催化剂含量煤基重质馏分加氢转化规律研究

Study on the Hydroconversion Law of Coal-Based Heavy Fractions with Different Catalyst Contents Based on an Improved Separation Method.

作者信息

Wang Yi, Tian Feng, Zhu Yonghong, Cui Louwei, Fan Xiaoyong, Du Chongpeng, Wang Feili, Zheng Huaan, Yang Yang, Li Dong

机构信息

School of Chemical Engineering, The Research Center of Chemical Engineering Applying Technology for Resource of Shaanxi, Northwest University, Xi'an, Shaanxi 710069, China.

Hydrocarbon High-Efficiency Utilization Technology Research Center, Yanchang Petroleum Co. Ltd., Xi'an, Shaanxi 710075, China.

出版信息

ACS Omega. 2023 Jun 15;8(25):22440-22452. doi: 10.1021/acsomega.3c00032. eCollection 2023 Jun 27.

Abstract

Heavy fractions (e.g., asphaltene and resin) can easily be subjected to physical aggregation and chemical coking reaction through molecular force in the process of lightweight processing and use of coal tar (CT), such that the normal processing and use can be affected. In this study, hydrogenation experiments were performed by regulating the catalyst to oil ratio (COR), while the heavy fractions of the hydrogenated products were extracted based on a novel separation method (e.g., the resin with a poor separation effect and rare existing research). The samples were analyzed through Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy, and thermogravimetric analysis. On that basis, the composition and structure characteristics of heavy fractions and the law of hydrogenation conversion were investigated. As indicated by the results, with the rise of the COR, the saturates, aromatics, resins, and asphaltenes (SARA) contents indicated the law of increasing the content of saturate, decreasing the content of other fractions, as well as sharply decreasing the content of asphaltene. Moreover, with the increase of the reaction condition, the relative molecular weight, the content of the hydrogen bonded functional groups and C-O groups, the carbon skeleton properties, the number of aromatic rings, and the stacking structure parameters were progressively reduced. In comparison with resin, asphaltene was characterized by large aromaticity and more aromatic rings, short and less alkyl side chains, as well as more complex heteroatoms on the surface of the heavy fractions. The results achieved in this study are expected to lay a solid basis for the relevant theoretical research and facilitate the industrial use process of CT processing.

摘要

在煤焦油(CT)轻质化加工和使用过程中,重质馏分(如沥青质和树脂)很容易通过分子力发生物理聚集和化学结焦反应,从而影响其正常加工和使用。本研究通过调节催化剂与油的比例(COR)进行加氢实验,同时基于一种新型分离方法(如分离效果较差且现有研究较少的树脂)对加氢产物的重质馏分进行萃取。通过傅里叶变换红外光谱、X射线光电子能谱、核磁共振光谱和热重分析对样品进行分析。在此基础上,研究了重质馏分的组成和结构特征以及加氢转化规律。结果表明,随着COR的升高,饱和烃、芳烃、树脂和沥青质(SARA)含量呈现出饱和烃含量增加、其他馏分含量降低以及沥青质含量急剧降低的规律。此外,随着反应条件的增加,重质馏分的相对分子量、氢键官能团和C-O基团含量、碳骨架性质、芳环数和堆积结构参数逐渐降低。与树脂相比,沥青质的特点是芳烃性大、芳环多、烷基侧链短且少,以及重质馏分表面的杂原子更复杂。本研究取得的结果有望为相关理论研究奠定坚实基础,并促进CT加工的工业应用过程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0bec/10308599/b84963177249/ao3c00032_0002.jpg

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