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化学学报
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化学学报 ›› 2007, Vol. 65 ›› Issue (17): 1757-1761. 上一篇    下一篇

研究论文

铜的表面氧在甲醇水蒸气重整反应中的作用

吴贵升1, 王宇红1, 毛东森1, 卢冠忠*,1, 曹勇2, 范康年2   

  1. (1上海应用技术学院化工系催化研究所 上海 200235)
    (2复旦大学化学系 上海 200433)
  • 投稿日期:2006-10-09 修回日期:2007-02-04 发布日期:2007-09-14
  • 通讯作者: 卢冠忠

The Role of Oxygen Species on the Surface of Copper in Methanol Steam Reforming

WU Gui-Sheng1; WANG Yu-Hong1; MAO Dong-Sen1; LU Guan-Zhong*,1; CAO Yong2; FAN Kang-Nian2   

  1. (1 Research Institute of Applied Catalysis, Department of Chemical Engineering, Shanghai In-stitute of Technology, Shanghai 200235)
    (2 Department of Chemistry, Fudan Univer-sity, Shanghai 200433)
  • Received:2006-10-09 Revised:2007-02-04 Published:2007-09-14
  • Contact: LU Guan-Zhong

PDF

853

被引次数

20 | 6

研究了Cu和ZrO2/Cu模型催化剂的甲醇水蒸气重整制氢的反应性能, 结果表明, 纯铜催化剂的反应初始活性随着还原温度的增加而显著降低, 并且在失活后的催化剂反应体系中通入少量的氧, 可恢复催化剂的活性. 相对于Cu, ZrO2/Cu催化剂的活性和稳定性显著增加. 催化剂的TPR, XPS以及原位FT-IR表征结果表明, 导致催化剂活性迅速降低的原因为催化剂表面氧物种的逐渐消耗. ZrO2在反应过程中可以稳定铜表面氧以及Cu＋物种, 从而显著提高了反应活性和稳定性.

关键词: Cu, ZrO2/Cu, 甲醇水蒸气重整, 表面氧

The performances of model catalysts such as Cu and ZrO2/Cu for methanol steam reforming (MSR) were investigated in the present work. It showed that the initial activity of Cu decreased with the rise of reduction temperature. Furthermore, Cu having lost its activity was reactivated through transient O2 pulse in the catalysis system. Compared with Cu, ZrO2/Cu showed very high activity and stability. The results of TPR, XPS and in-situ FT-IR indicated that the loss of catalytic activity was due to the gradual exhaustion of the surface oxygen on the copper. However, ZrO2 promoter stabilized the surface oxygen and Cu＋ species during the reaction process, then promoting the catalytic activity and stability.

Key words: Cu, ZrO2/Cu, methanol steam reforming, surface oxygen