物理化学学报 >> 2008, Vol. 24 >> Issue (06): 1085-1089.doi: 10.3866/PKU.WHXB20080630

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射频等离子体技术制备合成低碳醇用铜钴基催化剂

徐慧远; 储伟; 士丽敏; 张辉; 周俊   

  1. 四川大学化工学院, 成都 610065
  • 收稿日期:2008-01-14 修回日期:2008-03-20 发布日期:2008-06-03
  • 通讯作者: 储伟 E-mail:Chuwei65@yahoo.com.cn

Preparation of Copper-Cobalt Catalyst by Glow Discharge Plasma for Lower Alcohols Synthesis

XU Hui-Yuan; CHU Wei; SHI Li-Min; ZHANG Hui; ZHOU Jun   

  1. College of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China
  • Received:2008-01-14 Revised:2008-03-20 Published:2008-06-03
  • Contact: CHU Wei E-mail:Chuwei65@yahoo.com.cn

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摘要： 采用射频等离子体技术制备了CO加氢合成低碳醇用新型CuCo/ZrO2催化剂, 研究了等离子体气氛氮气、氢气和先氮气后氢气处理对催化剂结构和性能的影响, 并应用BET、XRD、XPS、TG和TPR技术对催化剂进行了表征. 与常规焙烧制得的样品相比, 射频等离子体技术制备的催化剂可有效抑制烃类生成, 提高总醇选择性, 大幅提高反应活性和低碳醇的时空收率. 表征结果显示, 等离子体技术使催化剂前驱体在低温下分解形成活性相, 显著提高了催化剂比表面积, 促进催化剂活性组分晶粒细化并提高其分散度, 催化剂表面的铜含量增加.

关键词: 铜钴基催化剂, 射频等离子体, 一氧化碳加氢, 低碳醇

Abstract: CuCo/ZrO2 catalysts for lower-alcohol synthesis from syngas were prepared by glow discharge plasma and conventional calcination method. The effects of plasma atmosphere(N2, H2 or first N2 then H2) on the catalyst structure and performance were investigated. These catalysts were characterized using BET, XPS, XRD, TG, and TPR techniques. The experimental results indicated that plasma treatment restrained effectively the production of hydrocarbon and enhanced the selectivity to total alcohols. Compared with the calcined sample, the plasma treated catalyst had higher activity and space time yield (STY). Characterization results showed that the catalyst precursor with plasma treatment was decomposed to active phase under low temperature and the specific surface area of catalyst was significantly improved. Meanwhile, the plasma treatment promoted the grain refining, dispersion of the active component and enrichment of copper on the catalyst surface.

Key words: Copper-cobalt based catalyst, Glow discharge plasma, CO hydrogenation, Lower alcohols