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盐酸溶液和水热脱铝HEU-1分子筛的表征及其催化裂解性能
  • ISSN号:0253-9837
  • 期刊名称:《催化学报》
  • 时间:0
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[1]中国石油大学(北京)重质油国家重点实验室,CNPC催化重点实验室,北京102249, [2]中海油新能源投资有限责任公司,北京100016, [3]中国科学院武汉物理与数学研究所,湖北武汉430071
  • 相关基金:国家重点基础研究发展计划(973计划,2010DFB40440); 国家自然科学基金(21176255,10979076); 国际科技与交流专项项目(2012CB215002,); 中石油科技创新基金(2010D-5006-0404)
中文摘要:

采用HCl溶液和/或水热处理HEU-1分子筛,利用X射线衍射、N2吸附-脱附、X射线荧光光谱、NH3程序升温脱附、吡啶吸附傅里叶变换红外光谱和铝固体核磁共振等对脱铝处理的HEU-1分子筛进行了表征,并考察了脱铝HEU-1分子筛上正己烷的催化裂解性能.结果表明,采用HCl溶液处理HEU-1分子筛,能有效脱除非骨架铝,可调变样品的弱酸中心;而水热处理HEU-1分子筛,能有效脱除骨架铝,可调变样品的强酸中心.水热处理和HCl溶液处理有效结合可以达到同时调变HEU-1分子筛的酸类型和酸密度的目的.脱铝HEU-1分子筛上正己烷催化裂解反应结果表明,氢转移反应被明显抑制,丙烯选择性提高.600°C水热处理后再用HCl溶液处理的HEU-1分子筛于625°C反应时丙烯选择性由未改性的21.9%提高到35.2%,活性稳定性也由不足10h提高到40h.

英文摘要:

A series of modified HEU-1 zeolites were prepared using hydrochloric acid treatment, hydrothermal treatment, and a combination of these. The parent and modified HEU-1 zeolites were characterized by X-ray diffraction, N2 adsorption-desorption isotherms, X-ray fluo- rescence, temperature-programmed desorption of ammonia, Fourier-transform infrared spectroscopy of adsorbed pyridine, and 27Al solid-state magic-angle spinning nuclear magnetic resonance techniques. The catalytic cracking performances of the modified HEU-1 zeo- lites were evaluated on a fixed-bed microreactor at 625 °C, atmospheric pressure, and an n-hexane weight hourly space velocity of 2.0 h?1. The results showed that extra-framework alumina could be removed by directly treating with hydrochloric acid, and framework alumina could be removed by hydrothermal treatment. Acidity characterization showed that the weak acid sites of HEU-1 zeolites could be adjusted using acid treatment, and the number of strong acid sites could be reduced using hydrothermal treatment. The framework nSi:nAl ratio was improved by using a combination of hydrothermal treatment and acid leaching. The acidities of the HEU-1 zeolites were adjusted and both the mesopore volume and external surface area were enhanced. In n-hexane cracking reactions, the dealuminated HEU-1 zeolite obtained by hydrothermal treatment for 4 h at 600 °C and then washing with hydrochloric acid exhibited the highest propylene production as a result of suppression of the hydrogen transfer reaction. At 625 °C, the selectivity for propylene on HEU-1(HT4-HCl) increased to 35.2% from 21.9%,and the lifetime of HEU-1(HT4-HCl) was also prolonged from not more than 10 to 40 h.

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期刊信息
  • 《催化学报》
  • 北大核心期刊(2011版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院大连化学物理研究所
  • 主编:李灿 张涛
  • 地址:大连市沙河口区中山路457号
  • 邮编:116023
  • 邮箱:chxb@dicp.ac.cn
  • 电话:0411-84379240
  • 国际标准刊号:ISSN:0253-9837
  • 国内统一刊号:ISSN:21-1195/O6
  • 邮发代号:8-93
  • 获奖情况:
  • 第三届国家期刊奖提名奖,中国科协精品科技期刊示范项目
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,美国剑桥科学文摘,美国科学引文索引(扩展库),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),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:19199