中空Zn/ZSM-5催化剂制备及其丙烷芳构化反应催化性能研究

徐国皓; 方佳璐; 罗帅; 胡永康

doi:10.12434/j.issn.2097-2547.20240356

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中空Zn/ZSM-5催化剂制备及其丙烷芳构化反应催化性能研究

- 中空Zn/ZSM-5催化剂制备及其丙烷芳构化反应催化性能研究
- Study on preparation of hollow Zn/ZSM-5 catalysts and their catalytic performances for propane aromatization
- 低碳化学与化工 2025: 1-6.
- 作者机构：
  
  1.阜阳师范大学化学与材料工程学院，安徽阜阳 236037
  2.阜阳师范大学安徽省绿碳化学重点实验室，安徽阜阳 236037
- 作者简介：
  
  徐国皓（1993—），博士，讲师，研究方向为低碳烷烃芳构化，E-mail：1447667520@qq.com。
- 基金信息：
  
  安徽省高校自然科学重点项目(2023AH050416);阜阳师范大学博士科研启动经费(2023KYQD0006);省级创新训练项目(S02410371077)
- DOI：10.12434/j.issn.2097-2547.20240356
  中图分类号： TQ426;O643
- 网络出版日期：2025-01-09，
  
  收稿日期：2024-08-28，
  
  修回日期：2024-12-04，
- 稿件说明：
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徐国皓,方佳璐,罗帅等.中空Zn/ZSM-5催化剂制备及其丙烷芳构化反应催化性能研究[J].低碳化学与化工,

XU Guohao,FANG Jialu,LUO Shuai,et al.Study on preparation of hollow Zn/ZSM-5 catalysts and their catalytic performances for propane aromatization[J].Low-carbon Chemistry and Chemical Engineering,
徐国皓,方佳璐,罗帅等.中空Zn/ZSM-5催化剂制备及其丙烷芳构化反应催化性能研究[J].低碳化学与化工, DOI：10.12434/j.issn.2097-2547.20240356.

XU Guohao,FANG Jialu,LUO Shuai,et al.Study on preparation of hollow Zn/ZSM-5 catalysts and their catalytic performances for propane aromatization[J].Low-carbon Chemistry and Chemical Engineering, DOI：10.12434/j.issn.2097-2547.20240356.

摘要

为提高常规分子筛催化剂的抗积炭性能，采用四丙基氢氧化铵（TPAOH）对ZSM-5进行二次晶化处理，进而制得了一系列Zn质量分数为2%的Zn/ZSM-5催化剂（Zn/ZSM-5(

)，

为二次晶化时间）。采用XRD、TEM和N

吸/脱附等对Zn/ZSM-5(

)进行了表征，并研究了其丙烷芳构化反应催化性能。结果表明，在脱硅重结晶过程中，ZSM-5内部的Si物种能够被OH

脱除，然后在四丙基铵阳离子（TPA

）作用下在ZSM-5表面重结晶，从而使催化剂形成中空结构。随着二次晶化时间延长，Zn/ZSM-5(

)的相对结晶度、介孔体积和壳层厚度逐渐增大，酸强度和酸量逐渐减小。在丙烷流量为5 mL/min、温度为600 ℃下反应4 h时，Zn/ZSM-5(36)表现出最优的催化性能，其丙烷转化率和芳烃（C

、C

和C

）选择性分别为80.0%和70.6%。此外，Zn/ZSM-5(36)表现出较好的抗积炭性能，反应4 h后其积炭量为1.8%。

Abstract

In order to improve the anti-coking performance of the conventional zeolite catalyst

a series of Zn/ZSM-5 catalysts (Zn/ZSM-5(

)

is the secondary crystallization time) with Zn mass

fraction of 2% were prepared by the secondary crystallization treatment of ZSM-5 using tetrapropylammonium hydroxide (TPAOH). Zn/ZSM-5(

) were characterized by XRD

TEM

absorption/desorption

etc. And the catalytic performances of the catalysts were investigated. The results show that during the desilication and recrystallization process

Si species inside ZSM-5 can be removed by OH

and then recrystallize on the surface of ZSM-5 under the action of tetrapropylammonium cation (TPA

)

so that the catalysts form a hollow structure. With the increase of secondary crystallization time

the relative crystallinities

mesoporous volumes and shell thicknesses of Zn/ZSM-5(

) increase gradually

while the acid strengths and acid amounts of the catalysts decrease gradually. Under the conditions of propane flow rate of 5 mL/min and temperature of 600 ℃ for 4 h

Zn/ZSM-5(36) exhibits the best catalytic performance with propane conversion rate and aromatic selectivity (C

and C

) of 80.0% and 70.6%

respectively. In addition

Zn/ZSM-5(36) has good anti-carbon deposition performance with carbon deposition amounts of 1.8% after reaction for 4 h.

关键词

中空结构二次晶化丙烷芳构化Zn/ZSM-5催化剂

Keywords

hollow structuresecondary crystallizationpropane aromatizationZn/ZSM-5 catalysts

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