催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (2): 230-236.DOI: 10.1016/S1872-2067(11)60327-6

• 研究快讯 • 上一篇    下一篇

以水热法合成的 ZrO2 负载 Au 催化剂的低温水煤气变换反应

张燕杰, 詹瑛瑛, 曹彦宁, 陈崇启, 林性贻, 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:2011-09-06 修回日期:2011-10-30 出版日期:2012-02-20 发布日期:2015-07-27

Low-Temperature Water-Gas Shift Reaction over Au/ZrO2 Catalysts Using Hydrothermally Synthesized Zirconia as Supports

ZHANG Yanjie, ZHAN Yingying, CAO Yanning, CHEN Chongqi, LIN Xingyi, ZHENG Qi*   

  1. National Engineering Research Center for Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
  • Received:2011-09-06 Revised:2011-10-30 Online:2012-02-20 Published:2015-07-27

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摘要： 采用一种简便的水热法合成了一系列 ZrO2, 并采用沉积-沉淀法制得相应 1.0% Au/ZrO2 催化剂, 在模拟甲醇重整气气氛下评价了它们的低温水煤气变换 (WGS) 反应催化性能. 结果发现, 于 150 oC 水热合成的 ZrO2 负载的 Au 催化剂活性最佳, 240 oC 反应时 CO 转化率达 87%, 明显高于相同反应条件下 Au 负载量较高的 Au/Fe2O3, Au/CeO2 及 Au/CeZrO4 催化剂. 采用 X 射线衍射、原子吸收光谱、N2 物理吸脱附及扫描电子显微镜等手段对样品进行了表征. 结果表明, Au/ZrO2 催化剂的总孔体积及平均孔径越大、圆形片状形貌越规整, 其低温 WGS 催化活性就越高.

关键词: 水热法, 水热合成温度, 金, 二氧化锆, 负载型催化剂, 水煤气变换反应

Abstract: Au/ZrO2 catalysts with a nominal gold loading of 1.0% were prepared by a deposition-precipitation method employing a series of ZrO2 samples synthesized by a convenient hydrothermal route as supports. These catalysts were evaluated for low-temperature water-gas shift reaction under a model reformed methanol gas atmosphere. The effect of the hydrothermal synthesis temperature of zirconia on the catalytic activity of Au/ZrO2 was investigated. The optimal hydrothermal synthesis temperature of ZrO2 was 150 °C. The corresponding catalyst offers a CO conversion of 87% at a reaction temperature of 240 °C, which is significantly higher than that of the previously reported Au/Fe2O3, Au/CeO2, and Au/CeZrO4 catalysts. The Au/ZrO2 catalysts were characterized by X-ray diffraction, atomic absorption spectrometry, N2-physisorption, and scanning electron microscopy. The results indicate that the catalytic performance of the Au/ZrO2 catalysts is mainly influenced by the morphology and pore structure of the ZrO2 that was hydrothermally synthesized at different temperatures. A uniform nanodisk morphology and increase in the pore volume and pore diameter of the ZrO2 particles lead to a higher catalytic activity of the Au/ZrO2 catalyst.

Key words: hydrothermal method, hydrothermal synthesis temperature, gold, zirconia, supported catalyst, water-gas shift reaction