芳烃重整油脱烯烃剂研究现状及展望

doi:10.19964/j.issn.1006-4990.2024-0233

Abstract

Abstract:

Benzene，toluene，xylene（BTX） is wildly used to synthetize high value products such as rubber，textile fibers，pharmaceuticals，and spices as an important raw materials of organic chemical.Recently，with the rapidly development of domestic petrochemical industry，the demand for BTX was increased by 2%~6% annually.In addition，the increasingly stringent environmental requirements for aromatics reforming technology promoted the continuous development of olefin removal catalyst for aromatic reforming oil.Based on these points，the research status and existed problems of two traditional olefin removal agents including the granular activated clay and selective hydrogenation refining catalysts were summarized firstly.Then，the catalysis，deactivation mechanism and industrial application status of emerging zeolite catalysts were emphatically introduced.Finally，the modification methods of zeolite were reviewed from three aspects：morphology and grain size regulation，pore structure controlment，and acidity adjustment.The design and development directions of molecular sieve catalysts for future industrial aromatics continuous reforming units were pointed out.

Key words: aromatics, trace olefins, deolefin agent, catalytic alkylation, zeolite

CLC Number:

O643.3

FAN Jingxin, LI Bin, HONG Luwei, HONG Meihua, GONG Xin. Research status and prospects of olefin removal catalyst from aromatic reforming oil[J]. Inorganic Chemicals Industry, 2025, 57(2): 14-25.

Figures/Tables 8

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分子筛催化剂结构特征	对脱烯烃反应的影响
孔道特征^［29-33］	当芳烃分子尺寸（约为0.7 nm）远大于分子筛孔道直径时，芳烃分子很难进入分子筛孔道，不能参与和烯烃的烷基化反应，因而孔道直径较小的ZSM-5分子筛脱烯烃效果最差
孔道特征^［29-33］	分子筛中窄且长的微孔孔道会带来较大的传质阻力，增加大分子产物烷基苯在催化剂上的停留时间；介孔和大孔结构则能够缩短晶内扩散路程，减少大分子传质扩散限制，提高分子筛酸中心的利用率，减缓分子筛的失活速率
酸性质^［34-35］	分子筛的中强B酸是烷基化反应的主要活性中心，L酸中心起辅助作用，B酸强酸位点过多会引发反应分子发生深度聚合，加速分子筛的失活；B酸和L酸的比例关系也会对分子筛的烷基化行为有一定影响
形貌与晶粒尺寸^［36-39］	随着分子筛晶粒尺寸的减小，晶体内部的孔道变短，有利于降低传质阻力，缩短大分子物质在分子筛活性位点上的停留时间，减少深度聚合或裂解反应的发生；独特层状结构的二维分子筛能够强化大分子物质在分子筛外表面的传输

分子筛催化剂	主要特点	有效改性方案
USY分子筛^［45-48］	孔道直径为0.9 nm，孔道适宜，总酸量高，初始活性较高，易结焦失活	1）通过脱铝改性后处理法增加分子筛介孔的比表面积和孔容；2）通过掺硼改性在分子筛晶内形成连通的介孔结构
Beta分子筛^［49］	晶粒尺寸为0.42~0.84 nm，孔道尺寸为0.64×0.76 nm，比表面积大，微孔结构丰富，强酸酸量高，初始活性较高，易结焦失活	通过脱铝改性后处理法增加分子筛介孔的比表面积和孔容，提高弱B酸酸量
ZSM-5分子筛^［50］	孔道尺寸为0.51 nm×0.55 nm，微孔结构丰富、酸性强，容易积炭且烯烃选择性较低	1）通过改性水热合成法减小晶粒尺寸，强化大分子物质的传质速率；2）通过软模板法，增加介孔孔容和外比表面积
MCM-22分子筛^［51］	晶粒尺寸为0.40 nm×0.59 nm，孔道尺寸为0.71 nm×1.81 nm，比表面积大，介孔结构丰富，弱酸含量高，结焦失活慢	1）铵离子交换，增加B酸酸量；2）骨架掺杂金属Ce，增加L 酸酸量

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Research status and prospects of olefin removal catalyst from aromatic reforming oil

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