催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (12): 1062-1066.

• 研究论文 • 上一篇    下一篇

完全液相法制备中原料配比对二甲醚合成催化剂结构和性能的影响

樊金串,吴慧,黄伟,石宇,谢克昌   

  1. 太原理工大学煤科学与技术教育部和山西省重点实验室, 山西太原 030024
  • 收稿日期:2007-12-25 出版日期:2007-12-25 发布日期:2007-12-25

Effect of Composition of Raw Materials on Structure and Dimethyl Ether Synthesis Activity of Cu-Zn-Al Catalyst Prepared by Complete Liquid Phase Method

FAN Jinchuan, WU Hui, HUANG Wei*, SHI Yu, XIE Kechang   

  1. Key Laboratory of Coal Science and Technology of Education Ministry and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2007-12-25 Online:2007-12-25 Published:2007-12-25

PDF

1077

被引次数

47

摘要： 利用完全液相法制备了Cu-Zn-Al双功能催化剂,考察了原料配比对催化剂结构和催化CO加氢合成二甲醚反应性能的影响,用XRD, N2吸附, XPS和H2-TPR等方法对催化剂进行了表征. 结果表明,在Cu-Zn-Al基二甲醚合成催化剂中, Zn和Al在催化剂表面的竞争富集是主要过程,增加投料中Cu的比例并不能显著增加Cu在催化剂表面的含量,因为在反应环境中, Al也会富集,并且在Cu含量高时富集得更快. 当投料组成为n(Cu)∶n(Zn)∶n(Al)=2∶1∶4时,催化剂的体相结构和表面性质最好(Cu晶粒度最小, Cu分散度最高,还原性能最佳,组分间相互作用最强,最可几孔径最大),催化剂的综合性能最好.

关键词: 铜, 锌, 铝, 双功能催化剂, 完全液相法, 一氧化碳, 加氢, 二甲醚

Abstract: The Cu-Zn-Al bifunctional slurry catalyst was prepared by a complete liquid phase method and characterized byX-raydiffraction,N2 adsorption,X-rayphotoelectron spectroscopy, and H2 temperature-programmed reduction. The effects of Al content and Cu/Zn molar ratio on the catalytic activity of the catalyst for dimethyl ether synthesis from syngas were investigated. The competitive enrichment of Zn and Al on the catalyst surface was dominating, and increasing the Cu content could not obviously increase the Cu amount on the catalyst surface. This is because Al was enriched faster on the catalyst surface than Cu under the reaction conditions in the case of the catalyst with higher Cu content. The catalyst withn(Cu)∶n(Zn)∶n(Al)=2∶1∶4 had the most favorable bulk structure and surface properties, such as the least Cu particle size, the highest dispersion degree, the excellent reductive character, the most strong interaction between metals, and the biggest probable pore radius. Therefore, this catalyst showed the best catalytic performance.

Key words: copper, zinc, aluminium, bifunctional catalyst, complete liquid phase method, carbon monoxide, hydrogenation, dimethyl ether