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丙烯直接环氧化Au/TiO2催化剂失活及再生研究

Research on the Deactivation and Regeneration of Au/TiO2 Catalyst for the Direct Epoxidation of Propylene

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【作者】 原宇航钱刚吴魏周兴贵袁渭康

【Author】 YUAN Yu-hang, QIAN Gang, WU Wei, ZHOU Xing-gui*, YUAN Wei-kang(State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China)

【机构】 华东理工大学化学工程联合国家重点实验室华东理工大学化学工程联合国家重点实验室 上海200237上海200237上海200237

【摘要】 采用沉积沉淀法制得Au/TiO2负载型催化剂,研究了该催化剂的丙烯气相直接环氧化合成环氧丙烷的反应性能,对新鲜、失活和再生后的催化剂进行TG-DTA、FT-IR、吡啶-IR、TEM以及活性评价等表征.研究结果表明,催化剂的失活是由于吸附在催化剂表面酸性Ti位上的环氧丙烷产物发生副反应生成了大分子沉积物.该沉积物存在着两种类型,其含有长碳烷基和酯基.催化剂再生实验表明在空气和H2中再生时活性恢复良好,而在N2中的再生效果则很差.

【Abstract】 Direct gas-phase epoxidation of propylene to PO in the presence of oxygen and hydrogen over the gold catalyst is an environmentally friendly process. In this paper, Au/TiO2 catalysts were prepared by the deposition-precipitation method. Fresh, deactivated and regenerated catalysts were characterized by HRTEM, FT-IR and DTA-TG. Results show that the fast deactivation of Au/TiO2 can be attributed to the deposition of some organic by-products on the catalyst. The deposit contains long-chain alkyl and ester groups. The activity of the catalysts can be fully restored after regeneration in air at 300 ℃; Regeneration in H2-N\-2 also can restore more than 95% of activity, indicating that H2 contributes to the desorption of the deposit; However, it was found that pure N2 plays poor role in the regenertion of deactivated catalysts, and only less than 50% of activity can be restored even under a high temperature of 500 ℃.

【基金】 国家自然科学基金资助项目(20276018);上海市重点学科资助项目.
  • 【文献出处】 分子催化 ,Journal of Molecular Catalysis , 编辑部邮箱 ,2005年03期
  • 【分类号】O643.361
  • 【被引频次】11
  • 【下载频次】265
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