摘要
为了将低价值、难裂解的正丁烷转化为高附加值的烯烃,采用浸渍法制备了La_(2)(SO_(4))_(3)/SiO_(2)系列催化剂,利用X射线衍射仪、物理吸附仪、扫描电子显微镜等仪器对系列催化剂进行了表征,考察了载体的比表面积、La_(2)(SO_(4))_(3)负载量(质量分数,下同)以及反应条件等因素对催化剂性质和反应性能的影响,同时与引入CeO_(2),TiO_(2),ZnO,ZrO_(2)等其他金属氧化物的催化剂进行了裂解性能对比。结果表明:载体SiO_(2)的比表面积越大,越有利于La_(2)(SO_(4))_(3)分散,烯烃(乙烯+丙烯,下同)收率随载体比表面积增大而增加,并随La_(2)(SO_(4))_(3)负载量的增加,先升高后降低,最佳负载量为10%,正丁烷转化率和烯烃收率分别为75.42%,43.91%;引入其他金属后10%La_(2)(SO_(4))_(3)/SiO_(2)的反应性能均出现下降,催化剂的反应活性由高到低依次为10%La_(2)(SO_(4))_(3)/SiO_(2),Ce-10%La_(2)(SO_(4))_(3)/SiO_(2),Zr-10%La_(2)(SO_(4))_(3)/SiO_(2),Ti-10%La_(2)(SO_(4))_(3)/SiO_(2),Zn-10%La_(2)(SO_(4))_(3)/SiO_(2),其中Zr的引入会影响La_(2)(SO_(4))_(3)形成;在反应温度650℃、进料质量空速0.36 h^(-1)的最佳工艺条件下,正丁烷转化率和烯烃收率分别为81.30%,44.90%。
In order to convert low value and difficult cracking n-butane into high value olefins,a series of La_(2)(SO_(4))_(3)/SiO_(2) catalysts were prepared by the impregnation method.The series of catalysts were characterized by instruments such as X-ray diffractometer,physical adsorption instrument,and scanning electron microscope.The effects of factors such as the specific surface area of the support,the loading amount of La_(2)(SO_(4))_(3)(mass fraction,the same below),and reaction conditions on the properties and cracking performance of the catalysts were investigated.Meanwhile,the cracking performance was compared with that of catalysts incorporating other metal oxides such as CeO_(2),TiO_(2),ZnO,and ZrO_(2).The results showed that the larger specific surface area of the support SiO_(2),the more favorable for the dispersion of La_(2)(SO_(4))_(3).The yield of olefins(ethylene+propylene,the same below)increased with the increase of the specific surface area of the support,and first increased and then decreased with the increase of the loading amount of La_(2)(SO_(4))_(3).The optimal loading amount was 10%,and the conversion rate of n-butane and the yield of olefins were 75.42% and 43.91%,respectively.After introducing other metals,the cracking performance of 10%La_(2)(SO_(4))_(3)/SiO_(2) all decreased.The cracking activity order of the catalysts from high to low was 10%La_(2)(SO_(4))_(3)/SiO_(2),Ce-10%La_(2)(SO_(4))_(3)/SiO_(2),Zr-10%La_(2)(SO_(4))_(3)/SiO_(2),Ti-10%La_(2)(SO_(4))_(3)/SiO_(2),Zn-10%La_(2)(SO_(4))_(3)/SiO_(2).Among them,the introduction of Zr would affect the formation of La_(2)(SO_(4))_(3).Under the optimal process conditions of a reaction temperature of 650℃ and a feed mass space velocity of 0.36 h^(-1),the conversion rate of n-butane and the yield of olefins were 81.30% and 44.90%,respectively.
作者
康豪
李建祥
王岳林
朱辰杰
任元珍
徐彩霞
刘明辉
张强
KANG Hao;LI Jian-xiang;WANG Yue-lin;ZHU Chen-jie;REN Yuan-zhen;XU Cai-xia;LIU Ming-hui;ZHANG Qiang(College of Chemistry and Chemical Engineering,State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China),Qingdao 266500,China)
出处
《石化技术与应用》
2025年第3期180-186,共7页
Petrochemical Technology & Application
基金
山东省重点研发计划(重大科技创新工程)资助项目(项目编号:2021ZLGX06)。
