噻吩在稀土离子改性Y型分子筛上吸附与催化转化研究  

Adsorption and catalytic conversion of thiophene on Y-type zeolites modified with rare-earth metal ions

作　　者：秦玉才[1,2] 高雄厚[3] 裴婷婷[2] 郑兰歌[2] 王琳[2] 莫周胜[1] 宋丽娟[1,2] 

机构地区：[1]中国石油大学(华东)化学化工学院,山东青岛266555 [2]辽宁石油化工大学辽宁省石油化工重点实验室,辽宁抚顺113001 [3]中国石油天然气股份有限公司石油化工研究院兰州化工研究中心,甘肃兰州730060

出　　处：《燃料化学学报》2013年第7期889-896,共8页Journal of Fuel Chemistry and Technology

基　　金：国家重点基础研究发展规划(973计划;2007CB216403);国家自然科学基金(20976077;21076100);中国石油天然气股份有限公司(10-01A-01-01-01)

摘　　要：以NaY、HY、液相Ce离子交换改性Y分子筛(L-CeY)和稀土离子改性超稳Y分子筛(HRSY-3)为研究对象,运用XRD、N2吸附、NH3-TPD和Py-FTIR表征样品的物化性能;采用原位红外光谱技术与程序升温脱附-同步质谱检测联用技术(TPD-MS)研究噻吩在活性中心上的吸附及催化转化行为。结果表明,稀土离子改性不改变分子筛晶体的基本结构但改变其精细结构,并形成一定的介孔,同时降低分子筛强酸位的强度,并生成与稀土离子物种有关的弱L酸位。REY与HY均可通过B酸中心的质子化作用活化噻吩,而稀土离子物种促进氢转移反应及低聚反应的进行,进而利于噻吩裂化反应的进行。Rare earth metal modified Y zeolites（L-CeY） and USY zeolites（HRSY-3） were characterized by XRD,N2 adsorption,NH3-TPD,and in-situ Py-FTIR;the adsorption and catalytic conversion behavior of thiophene on the modified zeolites were investigated by using the in situ FT-IR combined with TG-MS analysis.The results indicated that the original crystal structures of the zeolites remain unchanged after the modification with the rare earth metal ions;however,the modification results in the formation of partial mesoporous structure and weak Lewis acid sites related to the rare-earth ion species as well as certain decrease of the acidic strength of the strong acid sites.Thiophene molecules can be activated via protonization upon the Brnsted acid sites of the USY and HY zeolites;however,the rare earth metal ions are able to promote the hydrogen transfer and oligomerization reactions,which can then enhance the catalytic cracking of thiophene reactions.

关 键 词：噻吩 REY 吸附 氢转移 催化裂化 

分 类 号：TE626.21[石油与天然气工程—油气加工工程]