催化学报

催化学报 ›› 2008, Vol. 29 ›› Issue (12): 1242-1246.

• 研究论文 • 上一篇    下一篇

氟硅酸铵改性对HMCM-22酸性及双功能催化剂催化合成二甲醚性能的影响

毛东森1,夏建超2,陈庆龄2,卢冠忠1   

  1. 1 上海应用技术学院化学工程系应用催化研究所, 上海 200235; 2 中国石油化工股份有限公司上海石油化工研究院, 上海 201208
  • 收稿日期:2008-12-25 出版日期:2008-12-25 发布日期:2012-09-20

Effects of Ammonium Hexafluorosilicate Modification on Acidity of HMCM-22 and Catalytic Performance of CuO-ZnO-Al2O3/HMCM-22 for Dimethyl Ether Synthesis

MAO Dongsen1*, XIA Jianchao2, CHEN Qingling2, LU Guanzhong1   

  1. 1 Research Institute of Applied Catalysis, Department of Chemical Engineering, Shanghai Institute of Technology, Shanghai 200235, China; 2 Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208, China
  • Received:2008-12-25 Online:2008-12-25 Published:2012-09-20

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920

被引次数

3

摘要： 用氟硅酸铵对HMCM-22分子筛进行了改性处理,并采用氨程序升温脱附和吡啶吸附红外光谱法测定了其酸性. 结果表明,随着氟硅酸铵处理温度的提高, HMCM-22分子筛的B酸和L酸中心的酸量均逐渐减少. 以氟硅酸铵改性的HMCM-22分子筛为甲醇脱水活性组分与铜基甲醇合成活性组分(CuO-ZnO-Al2O3)组成双功能催化剂,在连续流动加压固定床反应器上考察了其对合成气直接制二甲醚反应的催化性能. 结果表明,对HMCM-22分子筛在适当温度(45 ℃)下进行氟硅酸铵改性,可使反应产物中烃类和CO2副产物的选择性下降,使目的产物二甲醚的选择性显著升高. 当氟硅酸铵处理温度过高(85 ℃)时, CO的转化率和二甲醚的选择性均大幅度降低.

关键词: HMCM-22分子筛, 氟硅酸铵, 改性, 甲醇脱水催化剂, 双功能催化剂, 合成气, 二甲醚

Abstract: HMCM-22 zeolite was modified with ammonium hexafluorosilicate at different t emperatures and used as an acidic component of the CuO-ZnO-Al2O3/HMCM-22 bifunctional catalyst for the direct synthesis of dimethyl ether (DME) from syng as. The modification at 45 ℃ (Cat F2) significantly enha nced DME selectivity. However, both CO conversion and DME selectivity were decre ased remarkably when the zeolite was treated at higher temperature (85 ℃, Cat F 3).

Key words: HMCM-22 zeolite, ammonium hexafluorosilicate, modification, methanol dehydration catalyst, bifunctional catalyst, syngas, dimethyl ether