催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (5): 842-849.DOI: 10.3724/SP.J.1088.2012.11117

• 研究论文 • 上一篇    下一篇

低温水煤气变换催化剂 Cu/ZrO2 的制备、表征与性能

阮春晓, 陈崇启, 张燕杰, 林性贻, 詹瑛瑛, 郑起*   

  1. 福州大学化肥催化剂国家工程研究中心, 福建福州 350002
  • 收稿日期:2011-11-16 修回日期:2011-12-26 出版日期:2012-05-09 发布日期:2012-05-09

Cu/ZrO2 Catalyst for Low-Temperature Water-Gas Shift Reaction: Preparation, Characterization and Performance

RUAN Chunxiao, CHEN Chongqi, ZHANG Yanjie, LIN Xingyi, ZHAN Yingying, ZHENG Qi*   

  1. National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
  • Received:2011-11-16 Revised:2011-12-26 Online:2012-05-09 Published:2012-05-09

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摘要： 以水热法制得的纯单斜相 ZrO2 为载体, 采用沉积沉淀法制备了一系列具有良好水煤气变换反应活性的 Cu/ZrO2 催化剂. 并通过 X 射线粉末衍射、N2 物理吸附、H2 程序升温还原、X 射线荧光元素分析、高分辨透射电镜和扫描电镜等手段考察了制备参数对 Cu/ZrO2 催化剂结构的影响, 探讨了其结构与性能的关系. 结果表明, CuO 负载量、沉淀温度、沉淀剂种类和焙烧温度均在一定程度上影响了催化剂活性组分的晶粒大小、分散状态、织构性质及载体与活性组分间的相互作用, 从而影响催化剂活性. 催化剂制备的适宜条件为: CuO 负载量 25%, 沉淀温度 65 oC, KOH 为沉淀剂, 在 H2 气氛 300 oC 焙烧 2 h.

关键词: 铜, 氧化锆, 水热法, 水煤气变换, 制备参数

Abstract: A series of Cu/ZrO2 catalyst samples with excellent catalytic performance for low-temperature water-gas shift (WGS) reaction were prepared by a two-step method. First, pure monoclinic ZrO2 support was prepared by hydrothermal synthesis, and then a certain amount of CuO was deposited on the support by deposition-precipitation. The catalyst samples were characterized by X-ray diffraction, N2-physisorption, H2 temperature-programmed reduction, X-ray fluorescence elemental analysis, high resolution transmission electron microscopy, and scanning electron microscopy, aiming to know the effect of preparation parameters on the catalytic performance of these samples. The relationship between their catalytic performance and structures was discussed. The crystalline size and dispersity of the Cu particles, texture of Cu/ZrO2 catalyst samples as well as the interaction between ZrO2 and Cu are greatly influenced by the preparation conditions, such as the CuO amount, precipitation temperature, precipitant and calcination temperature. And the optimal preparation parameters are ZrO2 loaded with 25% CuO, precipitation at 65 oC with KOH as precipitant, and calcination at 300 oC for 2 h purging with H2.

Key words: copper, zirconia, hydrothermal method, water-gas shift reaction, preparation parameter