载体改性对Ru/MCM-49催化剂金属粒径及分布的影响

石油炼制与化工 ›› 2023, Vol. 54 ›› Issue (11): 53-59.

载体改性对Ru/MCM-49催化剂金属粒径及分布的影响

张杰,张少平,李峰,郑家军,李瑞丰,李文林

太原理工大学化学工程与技术学院

收稿日期:2023-04-12 修回日期:2023-06-30 出版日期:2023-11-12 发布日期:2023-10-29
通讯作者: 李文林 E-mail:liwenlin@tyut.edu.cn
基金资助:
国家自然科学基金-中国海洋石油股份有限公司联合资助项目;山西省科技创新重点团队项目

EFFECT OF SUPPORT MODIFICATION ON METAL DISTRIBUTION AND STATE OF Ru/MCM-49 CATALYST

Received:2023-04-12 Revised:2023-06-30 Online:2023-11-12 Published:2023-10-29
Contact: Li Wenlin E-mail:liwenlin@tyut.edu.cn

摘要/Abstract

摘要： 以MCM-49分子筛为前体，经Ca、Mg金属改性后浸渍负载金属Ru，制备得到Ru-Ca/H-MCM-49和Ru-Mg/H-MCM-49催化剂，探索了碱土金属改性对Ru/H-MCM-49分子筛催化剂中Ru粒径大小的影响。对所制备催化剂进行了XRD、FT-IR、SEM、XPS、CO脉冲吸附和CO原位红外漫反射分析，并通过探针分子反应评价其催化性能。结果表明：改性金属对金属Ru在分子筛中的分布特性影响不大，两种催化剂上的Ru都主要分布于分子筛内部，但是Ca改性的Ru催化剂存在微孔堵塞现象；改性金属种类可以显著影响催化剂中Ru粒子的粒径，与Ca改性催化剂相比，Mg改性可以更好分散金属Ru，Ru粒子粒径约为2.7 nm，Ru-Mg/H-MCM-49具有更好的催化探针分子加氢性能。Ru-Mg/H-MCM-49催化剂对CO的吸附方式为多分子线性吸附，其对反应物分子的吸附和活化作用较强，有利于提高催化剂的加氢活性。

关键词: MCM-49分子筛, 金属粒径, 碱土金属, 原位红外漫反射

Abstract: Ru-Ca/H-MCM-49 catalyst and Ru-Mg/H-MCM-49 catalyst were prepared from MCM-49 zeolite modified by Ca and Mg and impregnated with Ru, and the effect of alkali metal modification on Ru particle size of Ru/H-MCM-49 zeolite catalyst was investigated. The catalysts were characterized by XRD, FT-IR, SEM, XPS, CO pulse adsorption, probe molecular reaction, and in situ CO-DRIFTS analysis. The results showed that the two modified metals had little effect on the distribution of Ru in the zeolite, and the Ru of both catalysts was distributed inside the zeolite, but the Ca modified Ru catalyst had the phenomenon of micro-porous blockage. The impregnated alkali metal species could significantly affect the size of Ru in the catalyst, and the support impregnated with Mg could better disperse Ru to form Ru nano-particles of about 2.7 nm, which showed higher probe molecular reaction performance. Catalyst Ru-Mg/H-MCM-49 adsorbed CO by linear multi-molecular adsorption, which had strong adsorption and activation effect on reactant molecules, and was beneficial to the hydrogenation activity of the catalyst.

Key words: MCM-49 zeolite, metal size, alkaline-earth metal, DRIFTS

张杰张少平李峰郑家军李瑞丰李文林. 载体改性对Ru/MCM-49催化剂金属粒径及分布的影响[J]. 石油炼制与化工, 2023, 54(11): 53-59.

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