催化、动力学与反应器Pt/Y催化剂催化FCC柴油加氢制备BTX

doi:10.11949/j.issn.0438-1157.20160795

摘要/Abstract

摘要：

利用Pt/Y催化剂，在固定床反应器中，温度380℃、压力3 MPa、氢油体积比1000及质量空速1.0 h^-1条件下，分别采用加氢处理的全馏分和轻馏分催柴为原料制备苯、甲苯和二甲苯（BTX），获得（C₆+C₇+C₈）芳烃的总选择性分别为9.4%和33.9%。对原料和液体产物进行的气相色谱和质谱分析表明，BTX主要经过重芳烃的加氢饱和、裂解等反应生成，中间物质为烷基苯、四氢萘、茚满及茚类等单环芳烃。通过对反应原料以及对反应前后催化剂的N₂吸脱附、NH₃-TPD、XRD衍射图谱、TG等物化性质的表征，分析催化剂失活的主要原因。即全馏分催柴原料中高含量的S、N化合物快速吸附造成了催化剂中毒，而轻馏分原料中S、N化合物在催化剂表面的缓慢积累覆盖活性位，造成催化剂逐渐失活。

关键词: 催化裂化柴油, 重芳烃, 分子筛, 催化剂, 固定床, 加氢, BTX

Abstract:

BTX was prepared by Pt/Y catalyzed hydrogenation of the whole or light fraction of hydrogenated FCC diesel in fixed bed reactor at reaction condition of temperature at 380℃, pressure at 3 MPa, volume ratio of V(H₂) over V(feed) at 1000, and WHSV at 1.0 h^-1. The overall selectivity of (C₆+C₇+C₈) arenes was 9.4% and 33.9% for the whole and light fraction of the hydrotreated FCC diesel, respectively. GC-MS study on feeds and liquid products showed that BTX were mainly produced through hydrogenation saturation and cracking of heavy arenes along with intermediate products of mononuclear aromatics such as alkylbenzenes, indane, tetralin, and indenes. By analysis of feeds, fresh and used catalysts via N₂-physisorption, NH₃-TPD, XRD, and TG, it was found that adsorption of high sulfur- and nitrogen- compounds in the whole fraction of FCC diesel quickly lead to catalyst toxication whereas slow accumulation and active site coverage on catalyst surface by sulfur- and nitrogen- compounds in the light fraction of FCC diesel gradually lead to catalyst deactivation.

Key words: FCC diesel, heavy aromatics, molecular sieves, catalyst, fixed bed, hydrogenation, BTX

中图分类号:

TQ028.8

周立坤, 于海斌, 葛庆峰, 范景新, 裴仁彦, 臧甲忠, 南军. 催化、动力学与反应器Pt/Y催化剂催化FCC柴油加氢制备BTX[J]. 化工学报, 2016, 67(11): 4623-4633.

ZHOU Likun, YU Haibin, GE Qingfeng, FAN Jingxin, PEI Renyan, ZANG Jiazhong, NAN Jun. Synthesis of BTX by Pt/Y catalyzed hydrogenation of FCC diesel[J]. CIESC Journal, 2016, 67(11): 4623-4633.

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