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铈改性对HZSM-5分子筛表面性质及其催化降解甲硫醇(CH_3SH)的研究
  • ISSN号:1000-4343
  • 期刊名称:《中国稀土学报》
  • 时间:0
  • 分类:O623.11[理学—有机化学;理学—化学]
  • 作者机构:昆明理工大学环境科学与工程学院,云南昆明650500
  • 相关基金:国家自然科学基金项目(U1402233,21267011和21367015); 云南省省级基金项目(KKSY201422060); 云南省教育厅面上基金项目(KKJA201422018)资助
中文摘要:

采用浸渍法制备了Ce改性的HZSM-5分子筛催化剂,考察Ce改性前后HZSM-5分子筛催化分解甲硫醇反应中的催化活性。通过XRD,BET,H_2-TPR,NH_3-TPD和CO_2-TPD等手段对其物化性能进行表征,结果表明:Ce改性后HZSM-5分子筛的结构没有被破坏,而Ce的引入可明显提高催化剂的还原性能,进而促进甲硫醇的催化分解;同时Ce的引入还能有效调控HZSM-5分子筛表面的酸碱性,可明显增加分子筛表面碱性中心的数量,从而显著提高催化分解甲硫醇的活性。此外,探讨了在350-650℃范围内焙烧温度对Ce改性HZSM-5分子筛表面性质及催化分解甲硫醇活性的影响。实验结果表明,在550℃焙烧获得的分子筛催化分解甲硫醇的效果最好。表征结果显示:当焙烧温度较低时,Ce与HZSM-5分子筛的相互作用较弱,所以分子筛催化分解甲硫醇的活性较差,随着焙烧温度的升高,分子筛的还原性能和酸碱性能均有所降低;当焙烧温度过高时,导致Ce O_2相互堆叠形成新的介孔孔道坍塌,降低其催化分解甲硫醇的活性。

英文摘要:

Rare earth Ce modified HZSM-5 catalysts were prepared by an incipient-wetness impregnation method,and the influence of different calcination temperatures on the activity of CH_3 SH catalytic decomposition were investigated. The physical and chemical properties of the synthesized catalysts were characterized by XRD,BET,H_2-TPR,NH_3-TPD and CO_2-TPD. The results showed that doping of Ce would not destroy the framework structure of HZSM-5,while the existence of Ce O_2 phase in HZSM-5 catalysts improved the reducibility of the catalysts,which should be in favor of the catalytic decomposition of CH_3 SH. Furthermore,the introduction of Ce could effectively regulate the acidity and basicity,which may affect the catalytic activity of decomposition of CH_3 SH. The effect of calcination temperature between 350 and 650 ℃ was investigated on the surface properties and catalytic activity in decomposition of CH_3 SH of these catalysts. The sample HZSM-5 calcined at 550 ℃ exhibited the best catalytic activity in decomposition of CH_3 SH. The characterization results indicated that when the calcination temperature was low,the interaction between cerium and HZSM-5 zeolite is weaker,which decreased the activity of catalytic decomposition of CH_3 SH. With the increase of calcination temperature,the reducibility and the acid-base properties of the catalysts were decreased. When the calcination temperature was higher,resulting in Ce O_2 mutually stacked to form new mesoporous pore collapse,which should reduce its catalytic decomposition activity of CH_3 SH.

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期刊信息
  • 《中国稀土学报》
  • 中国科技核心期刊
  • 主管单位:中国科学技术协会
  • 主办单位:中国稀土学会
  • 主编:徐光宪
  • 地址:北京新街口外大街2号
  • 邮编:100088
  • 邮箱:jrechina@263.net
  • 电话:010-62014832
  • 国际标准刊号:ISSN:1000-4343
  • 国内统一刊号:ISSN:11-2365/TG
  • 邮发代号:2-612
  • 获奖情况:
  • 优秀科技期刊奖,中国科协择优资助期刊,中国科协期刊奖
  • 国内外数据库收录:
  • 美国化学文摘(网络版),荷兰文摘与引文数据库,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),中国北大核心期刊(2000版)
  • 被引量:12811