物理化学学报 >> 2016, Vol. 32 >> Issue (2): 527-535.doi: 10.3866/PKU.WHXB201512033

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原位晶化FCC催化剂传质性能的频率响应法辨析

秦玉才1,高雄厚2,*(),石利飞1,张莉2,段林海1,宋丽娟1,*()   

  1. 1 辽宁石油化工大学,辽宁省石油化工催化科学与技术重点实验室, 辽宁抚顺 113001
    2 中国石油天然气股份有限公司,石油化工研究院兰州化工研究中心, 兰州 730060
  • 收稿日期:2015-08-27 发布日期:2016-01-30
  • 通讯作者: 高雄厚,宋丽娟 E-mail:gaoxionghou@petrochina.com.cn;lsong56@263.net
  • 基金资助:
    国家自然科学基金(21076100, 21376114);中国石油天然气股份有限公司(10-01A-01-01-01);辽宁省高校创新团队资助项目

Discrimination of the Mass Transfer Performance of In situ Crystallization FCC Catalysts by the Frequency Response Method

Yu-Cai QIN1,Xiong-Hou GAO2,*(),Li-Fei SHI1,Li ZHANG2,Lin-Hai DUAN1,Li-Juan SONG1,*()   

  1. 1 Key Laboratory of Petrochemical Catalytic Science and Technology of Liaoning Province, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China
    2 Lanzhou Petrochemical Research Center, Petrochemical Research Institute, Petro China Company Limited, Lanzhou 730060, P. R. China
  • Received:2015-08-27 Published:2016-01-30
  • Contact: Xiong-Hou GAO,Li-Juan SONG E-mail:gaoxionghou@petrochina.com.cn;lsong56@263.net
  • Supported by:
    the National Natural Science Foundation of China(21076100, 21376114);China National Petroleum Corporation(10-01A-01-01-01);Innovation Team of Liaoning Province Colleges, China

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摘要：

以苯为探针分子,采用频率响应(FR)技术和智能重量分析仪(IGA)研究了原位晶化流化催化裂化(FCC)催化剂上的传质行为。结合N2吸附和扫描电镜(SEM)剖析所得织构性质数据,并与传统半合成FCC催化剂以及稀土改性Y分子筛传质性能进行对比,结果表明原位晶化FCC催化剂所具有的独特纳米化和高度分散的分子筛组分分布状态,显著改善了基质大孔/介孔结构与分子筛微孔孔道的贯通性,削弱了分子筛孔道与基质界面间的传质阻力,从而优化了成型催化剂颗粒的传质性能。本研究再次证实了频率响应技术可以检测和辨析多孔催化材料体系中发生的复杂吸附-扩散过程,是一种有效的多级孔催化材料传质性能的研究手段。

关键词: 频率响应技术, 原位晶化, 流化催化裂化催化剂, 传质过程, 孔道贯通性

Abstract:

Mass transfer behaviors of benzene in an in situ crystallization fluid catalytic cracking (FCC) catalyst were measured and discriminated by the frequency response (FR) method and an intelligent gravimetric analyzer (IGA). The texture properties of the FCC catalysts were analyzed by N2 adsorption and scanning electron microscope (SEM). By comparison with the mass transfer performance of a semi-synthetic FCC catalyst, as well as a zeolite Y, the results show that the in situ crystallization FCC catalyst has excellent and improved mass transfer behavior over the semi-synthetic FCC catalyst and that it reduces the mass transfer resistance between the interface of zeolite crystal and substrate, which can be attributed to the excellent porous connectivity of the former with the unique accumulation state of the highly dispersed nanosized Y zeolite crystals. It has been demonstrated that the FR technique can be used to measure and distinguish the complex mass transport processes in hierarchical porous catalytic materials.

Key words: Frequency response method, In situ crystallization, Fluid catalytic cracking catalyst, Mass transfer process, Porous connectivity