Silicalite-1分子筛的低成本合成及其MTP催化性能  

Synthesis and catalytic MTP performance of Silicalite-1 zeolite with low cost

作　　者：陶金泉 贾亦静 白天瑜 姚荣鹏 黄文斌 崔岩[2] 周亚松[1] 魏强[1] TAO Jinquan;JIA Yijing;BAI Tianyu;YAO Rongpeng;HUANG Wenbin;CUI Yan;ZHOU Yasong;WEI Qiang(College of Chemical Engineering and Environment,China University of Petroleum(Beijing),Beijing 102206,China;PetroChina Petrochemical Research Institue,Beijing 102206,China)

机构地区：[1]中国石油大学(北京)化学工程与环境学院,北京102206 [2]中国石油天然气股份有限公司石油化工研究院,北京102206

出　　处：《化工进展》2025年第3期1550-1558,共9页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(22078360)。

摘　　要：分子筛的高效、环保和合成廉价在学术及工业应用领域都具有重要的意义。传统水热合成法中非有机胺体系因其弱导向性和杂晶相的竞争生长导致纯硅MFI分子筛(Silicalite-1)的合成极具挑战性。本文在甲醇体系中成功合成出Silicalite-1分子筛,并重点考察了水热合成过程中甲醇的作用和晶化条件(水硅比、醇硅比等)对分子筛合成的影响。使用蒙特卡罗模拟、X射线衍射(XRD)、扫描电子显微镜(SEM)、热重(TG)、N_(2)-吸附脱附和NH_(3)-程序升温脱附(NH_(3)-TPD)等方法进行了计算与表征。结果表明:引入晶种可以明显改善甲醇体系在晶化初期成核困难的问题,当晶种投入量为3%(质量分数)、醇硅比为3.3时可以直接合成出高结晶度的纯相Silicalite-1分子筛,该分子筛表现出优异的甲醇制丙烯(MTP)反应催化活性。最后,本文提出的Silicalite-1分子筛低成本合成策略具有显著的科研价值和工业化应用前景。The efficient,environmentally friendly,and cost-effective synthesis of zeolites holds significant importance in both academic and industrial applications.Traditionally,the synthesis of pure silicon MFI zeolite(Silicalite-1)through hydrothermal methods employing non-organic amine systems posed substantial challenges due to weak directing abilities and competitive growth of impure phases.In this study,Silicalite-1 zeolite was successfully synthesized in a methanol system,and particular attention was paid to the role of methanol and the crystallization conditions(water-to-silica ratio,alcohol-to-silica ratio,etc.)during the hydrothermal synthesis process.Computational and characterization techniques such as Monte Carlo simulations,XRD,SEM,TG,N_(2)adsorption-desorption,and NH_(3)-TPD were employed.The results indicated that the introduction of seed crystals significantly improved the initial nucleation difficulties in the methanol system;a pure phase of Silicalite-1 with high crystallinity was directly synthesized when the seed crystal input was 3%and the alcohol-to-silica ratio was 3.3,showing excellent catalytic activity in the MTP reaction.Lastly,the low-cost synthesis strategy for Silicalite-1 proposed in this paper has notable research value and industrial application prospects.

关 键 词：分子筛 合成 蒙特卡罗模拟 催化剂 稳定性 

分 类 号：TQ221.2[化学工程—有机化工] TQ426