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化学学报
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化学学报 ›› 2009, Vol. 67 ›› Issue (23): 2739-2744. 上一篇    下一篇

研究论文

Cu/SiO2催化剂制备方法对其草酸二甲酯催化氢解性能的影响

陈梁锋，朱 渊，刘晓钰，裴 燕，乔明华，沈 伟，徐华龙*，范康年   

  1. (复旦大学化学系 分子催化和功能材料重点实验室 上海 200433)
  • 投稿日期:2008-12-15 修回日期:2009-04-29 发布日期:2009-08-10
  • 通讯作者: 乔明华 E-mail:mhqiao@fudan.edu.cn
  • 基金资助:

    “973”国家重点基础研究发展规划资助项目（2006CB202502），国家自然科学基金资助项目（20673025，20803011）霍英东教育基金会资助项目（104022）和上海市科委资助项目（06JC14009，07ZR14007）

Cu/SiO2 Catalysts Prepared by Different Methods for Hydrogenolysis of Dimethyl Oxalate to Ethylene Glycol

Chen, Liangfeng，Zhu, Yuan，Liu, Xiaoyu，Pei, Yan，Qiao, Minghua* Shen, Wei，Xu, Hualong*，Fan, Kangnian   

  1. (Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433)
  • Received:2008-12-15 Revised:2009-04-29 Published:2009-08-10

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以化学吸附水解法、蒸氨法和浸渍法制备了Cu/SiO2催化剂, 并用于草酸二甲酯氢解制备乙二醇的反应. 发现用化学吸附水解法制备的催化剂具有最高的催化活性和乙二醇选择性, 乙二醇得率可达92.6%. 对还原前后不同方法制备的催化剂进行表征发现, 浸渍法制备的催化剂中Cu物种不能很好地得到分散, 因此活性较差. 蒸氨法和化学吸附水解法能较好地分散Cu物种. 由于化学吸附水解法制备的催化剂的Cu0表面积较蒸氨法的大, 且Cu＋表面积相当, 故活性高于蒸氨法制备的催化剂.

关键词: Cu/SiO2, 制备方法, 草酸二甲酯, 氢解, 乙二醇

Cu/SiO2 catalysts have been prepared by the chemisorption-hydrolysis (CH), ammonia evaporation (AE) and wetness impregnation (WI) methods, and evaluated in gas phase hydrogenolysis of dimethyl oxalate (DMO) to ethylene glycol (EG). The Cu/SiO2 catalyst prepared by the CH method showed the highest hydrogenolysis activity and selectivity to EG, giving an EG yield of 92.6%. Characterizations disclosed that Cu species were poorly dispersed on the catalyst prepared by the WI method, which accounts for its poor activity. CH and AE methods could well disperse Cu species, but the CH method resulted in higher Cu0 surface area and comparable Cu＋ surface area as compared to the AE method. As a result, the Cu/SiO2 catalyst prepared by the CH method exhibits the higher hydrogenolysis activity than that by the AE method.

Key words: Cu/SiO2, preparation method, dimethyl oxalate, hydrogenation, ethylene glycol