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柠檬酸改性Hβ分子筛上的苯与丙烯烷基化反应
  • ISSN号:0253-2409
  • 期刊名称:《燃料化学学报》
  • 时间:0
  • 分类:O643.32[理学—物理化学;理学—化学]
  • 作者机构:[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001, [2]中国科学院研究生院,北京100039
  • 相关基金:国家自然科学基金(20473110);国家重点基础研究发展规划(973计划,G2000IM8010).
中文摘要:

研究了柠檬酸改性对Hβ分子筛上苯与丙烯烷基化反应性能的影响。通过比较分析改性前后催化剂寿命、二异丙苯选择性及其异构体组成分布等的变化。结果表明,二异丙苯的选择性及各异构体的分布与催化剂的酸密度和酸强度有关;较高酸密度和酸强度有利于烷基转移反应的进行,但却加快了催化剂的失活。柠檬酸改性处理可调节Hβ分子筛的酸密度和酸强度,改善苯烷基化的催化反应性能。经0.50mol/L的柠檬酸处理后,Hβ催化剂的寿命比原来延长30%,正丙苯的质量分数减少90%。

英文摘要:

Carrying out the alkylation of benzene with propene over zeolites ( especially ZSM-5, Y, mordenite, and β instead of AlCl3 or phosphoric acid as catalysts can be an environmentally friendly and noncorrosive process without the release of acidic catalyst components. Performing the reaction under supercritical conditions is effective to alleviate the catalyst deactivation caused by the carbonaceous deposition. However, it is still necessary to modify the zeolites to improve the catalyst life time and to decrease the contents of by-products that may have undesired effects on the quality of subsequent products. Therefore, in this work, the properties of Hβ zeolite modified with citric acid and its catalytic behaviours on the alkylation of benzene with propene under supercritical conditions were investigated. The results indicate that the catalytic behaviour of Hβ zeolite like catalyst life, n-propylbenzene content, di-isopropylbenzene selectivity and the isomers distribution is related to the acid strength and density of acidic sites of the catalyst, which can be modified with the treatment of citric acid. High density of acidic sites with high acid strength is favorable for the transalkylation, but aggravates the catalyst deactivation, which is mainly caused by the blocking of pore structure due to coke deposition. The concentration of citric acid has a significant influence on the properties of treated Hβ catalysts. Low concentration of citric acid may enhance the acid strength and density, while high concentration may result in the decrease of acid density and the distortion of pore structure. Hβ treated with the citric acid solution of 0.5 mol/L owns high density of weak and moderate acidic sites; by carrying the alkylation over it, the catalyst life prolonged about 30 % and n - propylbenzene content decreased about 90% in comparison with that over the untreated Hβ catalyst.

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期刊信息
  • 《燃料化学学报》
  • 中国科技核心期刊
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院山西煤炭化学研究所
  • 主编:王建国
  • 地址:太原市桃园南路27号中国科学院山西煤炭化学研究所
  • 邮编:030001
  • 邮箱:rlhx@sxicc.ac.cn
  • 电话:0351-2025214
  • 国际标准刊号:ISSN:0253-2409
  • 国内统一刊号:ISSN:14-1140/TQ
  • 邮发代号:22-50
  • 获奖情况:
  • 获国家优秀期刊三等奖,中科院优秀期刊二等奖,华北优秀期刊奖和山西省一级期刊,《中国学术期刊(光盘版)检索与评价资料规范》优秀奖,2001年获新闻出版总署授予的“中国期刊方阵“双效...,连续十五年获山东省一级期刊
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),波兰哥白尼索引,荷兰文摘与引文数据库,美国工程索引,美国剑桥科学文摘,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:14785