肖天存,王海涛,苏继新,陈方,鹿玉理,安立敦,王弘立.凝胶中硅含量对SAPO-5分子筛合成及其性能的影响[J].分子催化,1998,(5):367-374 |
凝胶中硅含量对SAPO-5分子筛合成及其性能的影响 |
Effect of Silicon Content in Gel Mixture on the Structure and Acid Catalytic Performance of SAPO 5 Molecular Sieve |
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DOI: |
中文关键词: SAPO-5分子筛,硅含量,结构,催化活性 |
英文关键词:SAPO 5 molecular sieve, Si content, Structure, Catalytic activity, |
基金项目:山东省优秀青年科学家奖励基金 |
肖天存 王海涛 苏继新 陈方 鹿玉理 安立敦 王弘立 |
山东大学环境工程系,中国科学院兰州化学物理研究所 |
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中文摘要: |
通过改变反应物凝胶中的硅含量,用水热法合成了系列SAPO-5分子筛,并用XRD、SEM和MASNMR分别研究了不同硅含量的分子筛结构和形貌.以正己烷的催化裂解为模型反应,用微反色谱研究了不同硅含量的SAPO-5分子筛的催化性能.结果表明,分子筛骨架中的硅含量随反应物中硅含量的增加而增加;硅开始进入SAPO-5分子筛骨架时,是以取代单个磷原子而进行的;当反应物中硅含量较高时,硅进入分子筛骨架是通过两个硅原子取代一对铝和磷原子,从而在SAPO-5中形成富硅区.硅进入分子筛骨架,虽然未改变分子筛的晶体结构,但改变了分子筛的晶形晶貌.SAPO-5分子筛中存在3种酸中心,即弱酸、中强酸和强酸中心.在正己烷催化裂解中,较低温度时,催化活性中心主要是中强酸中心;当反应温度较高时,弱酸中心也可充当活性中心.在强酸中心上易发生结炭现象. |
英文摘要: |
A series of SAPO 5 molecular sieves has been synthesized by changing Si content in reaction mixture. XRD, SEM and MAS NMR were employed to characterize the structure and morphology of SAPO 5 with different Si contents. The acid catalysis of SAPO 5 catalysts was evaluated by micro reactor chromatography. The results show that the Si content in the framework of SAPO 5 increases with the Si content in gel mixture. Si atoms start to enter the framework of SAPO 5 by replacing single P atom in the framework of AlPO 4 5. When the Si content is high in gel mixture Si atoms start to replace a pair of P and Al in the framework of AlPO 4 5, and thus the silicon rich zone is formed in SAPO 5. Although the structure of SAPO 5 can not be changed by the entrance of Si atoms into the framework, the morphology of SAPO 5 is changed. In SAPO 5 catalyst, there are three types of acid sites, i.e weak, medium strong and strong acid sites. In the catalytic cracking reaction of n hexane , at lower reaction temperature the medium and strong acid active sites play the main role; while at higher temperature, the weak acid sites can also play some role. During cracking reaction, coke is easily to be formed on the strong acid sites. |
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