H-SAPO-34分子筛催化醇类转化的差异性研究

Investigation on the Differences of the Alcohols Conversion over H-SAPO-34 Zeolite

本文研究了H-SAPO-34催化甲醇和丁醇转化反应及其产物分布的差异,结合气相色谱-质谱(GC-MS)联用、^(13)C交叉极化魔角旋转核磁共振(^(13)C CP MAS NMR)技术捕获了反应过程中生成的重要反应中间物种.甲醇转化过程以乙烯、丙烯和丁烯为主要产物;而丁醇转化过程中主要产物是丁醇脱水生成的丁烯,反应初期以丙烯和丁烯作为主要产物.两种醇类转化均以低碳烯烃作为主要产物,且存留物种和^(13)C CP MAS NMR分析均观察到芳烃物种,说明H-SAPO-34催化甲醇和丁醇转化存留在催化剂上的有机物种相近.虽然起始于不同的醇类反应,但H-SAPO-34上限域空间的酸催化环境都能引导甲醇和丁醇制取低碳烯烃的反应过程.

In this paper,the conversion of methanol and butanol and the differences in product distribution over H-SAPO-34 were investigated.Some important reaction intermediates were captured during the reaction process by using gas chromatography-mass spectrometry(GC-MS)and ^(13)C cross polarization magic angle spinning nuclear magnetic resonance(^(13)C CP MAS NMR)spectroscopy.In the methanol conversion process,ethene,propene and butene are the main products,while in the butanol conversion process,butanol is mainly dehydrated to form butene,and propene and butene are the main products in the initial stage.Light olefins are generated from both methanol and butanol conversion over H-SAPO-34.Furthermore,the aromatic species were observed in both retained species analysis and ^(13)C CP MAS NMR,indicating that similar organic species confined in the H-SAPO-34 during the conversion of alcohols.Starting from different kinds of alcohols,the acid-catalysis environment in the confined space of H-SAPO-34 can catalyze the methanol and butanol conversion to produce light olefins.