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液相晶化法合成SAPO系列分子筛的研究

Study on the Synthesis of SAPO Molecular Sieve with Liquid-phase Crystallization Method

【作者】 王晓梅

【导师】 张秀成;

【作者基本信息】 西北大学 , 化学工程, 2008, 硕士

【摘要】 本文介绍了SAPO-34分子筛的开发意义和国内外研究现状,并对SAPO-34分子筛的合成方法、原料的影响进行了深入的研究。本文采用一种新的方法——液相晶化法合成了SAPO-34分子筛和SAPO-20分子筛;采用自动吸附仪、XRD、SEM和FT-IR等手段对合成的SAPO-34和SAPO-20分子筛样品进行了表征;采用液相晶化法合成SAPO-34分子筛时,晶化温度、晶化时间和原料的纯度对分子筛有重大影响;140~180℃和96~120h是适宜的晶化温度和晶化时间;硅源的纯度对合成的SAPO-34分子筛的结晶影响最大。对于SAPO-20分子筛,研究了干胶颗粒的大小、干胶中模板剂的加入、模板剂加入的顺序和HF的加入对分子筛的影响。其中,干胶的颗粒越小,越容易合成出结晶度高的SAPO-20分子筛;在干胶中加入吗啉模板剂对分子筛的结晶影响不是很大;加入HF能提高分子筛的结晶度。硅源、铝源、磷源和水的比例相同,模板剂的种类不同将会合成出完全不同的分子筛,以吗啉为模板剂合成出的是SAPO-20分子筛,以吗啉和四乙基氢氧化铵为模板剂合成的是SAPO-34分子筛。对不同的原料合成的SAPO-34分子筛进行MTO催化性能的测试,结果表明,在320℃时,部分分子筛样品的甲醇转化率达到95%以上,乙烯丙烯的总选择性达到78%以上。

【Abstract】 The research meaning of SAPO-34 molecular sieve and methanol-to-Olefins at home and abroad were reviewed.The synthetic method and the effect to SAPO-34 molecular sieve of the purity of raw materials were studied in this article.A series of SAPO-34 molecular sieve samples and SAPO-20 molecular sieve samples were synthesized with a new method that named liquid-phase crystallization method.SAPO-34 and SAPO-20 molecular sieve samples have been characterized by specific surface area,XRD,SEM and FT-IR techniques.Crystallization temperature,crystallization time and the purity of alumina,silica sol and template have important effect to the crystallization of SAPO-34 molecular sieve.140-180℃and 96-120h were suitable crystallization temperature and crystallization time of SAPO-34 molecular sieve synthesized with liquid-phase crystallization method.The purity of silica sol was the seriousest effect to the crystallization of SAPO-34 molecular sieve.The effect to SAPO-20 molecular sieve of the size of dry gel granule,the time of adding template and HF were studied.The result showed the small size dry gel granule was advantageous to the crystallization of SAPO-20 molecular sieve.Add some template to dry gel when making it,have little effect to SAPO-20 molecular sieve.HF would improved the crystallization of SAPO-20 molecular sieve.The raw materials composition were same,only the quantity of template was changed,different molecular sieve were synthesized.SAPO-20 molecular sieve samples have been synthesized by using Morpholine as template,while SAPO-34 molecular sieve samples have been synthesized by using Morpholine and tetraethylammonium hydroxide (TEAOH) as template.The SAPO-34 molecular samples synthesized with different purity sources with liquid-phase crystallization method were investigated by MTO process.The resulte showed at 320℃,the conversion of CH3OH exceeded 95%,the overall selection of ethylene and propylene is more than 78%.

  • 【网络出版投稿人】 西北大学
  • 【网络出版年期】2008年 08期
  • 【分类号】O643.36
  • 【被引频次】9
  • 【下载频次】365
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