石油炼制与化工

• 基础研究 •    下一篇

模板剂对SAPO-34的合成、性质及催化性能的影响

李黎声 李军 张凤美   

  1. 石油化工科学研究院 长岭炼化公司催化剂厂,湖南 岳阳 石油化工科学研究院
  • 收稿日期:2007-08-21 修回日期:1900-01-01 出版日期:2008-04-12 发布日期:2008-04-12
  • 通讯作者: 李黎声

EFFECT OF TEMPLATE ON THE SYNTHESIS, CHARACTERISTICS AND CATALYTIC PERFORMANCE OF SAPO-34

Li lisheng jun li fengmei zhang   

  • Received:2007-08-21 Revised:1900-01-01 Online:2008-04-12 Published:2008-04-12
  • Contact: Li lisheng

摘要: 分别以TEA、DEA和TEA+DEA为模板剂进行了SAPO-34分子筛的合成。以TEA为模板剂只能得到CHA/AEI的共生结构产物;以DEA为模板剂能够得到纯相的SAPO-34,但是合成条件比较苛刻;以DEA+TEA为模板剂时,当DEA的量大于总模板剂量的一半时,得到的是纯相SAPO-34。研究了TEA和DEA的不同比例对于晶化产物物化性质的影响。模板剂中DEA的比例的增加,晶化产物中的硅含量增加,孔体积和比表面不断减小,晶粒逐渐增大,酸中心数不断减少,酸强度有所减弱。对合成的分子筛的MTO催化性能进行了研究。随着模板剂中DEA比例的增加, MTO反应产物中乙烯收率降低,而丙烯收率提高,C2=+C3=的选择性逐渐增加。

关键词: 磷酸硅铝, 分子筛, 模板剂, 二乙胺, 三乙胺, 合成

Abstract: Using various templates, triethylamine (TEA), diethylamine (DEA) and TEA+DEA, SAPO-34 molecular sieve was synthesized, respectively. The test results showed that pure SAPO-34 crystal phase (CHA) could not be formed when using TEA as template, only CHA/AEI intergrowth crystal was formed. When using DEA as template, pure CHA phase was obtained under narrow synthesis conditions. SAPO-34 with pure CHA structure could be easily synthesized when using TEA+DEA mixed template having a DEA/TEA ratio of over 1. The effects of templates on the physicochemical properties and catalytic performance of the obtained products were studied. It was found that with the increase of DEA proportion in the mixed template, the content of silicon in the obtained molecular sieve increased, the specific surface area and pore volume decreased, the crystal size increased, the number of active acid sites decreased and with acid strength weaken. When the obtained SAPO-34 molecular sieve samples were used as catalysts in the methanol-to-olefin (MTO) reaction, it was observed that with the increase of DEA proportion in the mixed template, the ethylene yield decreased, propylene yield increased, and the selectivity of C2=+C3= increased gradually.

Key words: silicoaluminophosphate, molecular sieve, template, diethylamine, triethylamine, synthesis