Mesoporogen‐Free Synthesis of Hierarchical SAPO‐34 with Low Template Consumption and Excellent Methanol‐to‐Olefin Conversion,ChemSusChem

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Mesoporogen‐Free Synthesis of Hierarchical SAPO‐34 with Low Template Consumption and Excellent Methanol‐to‐Olefin Conversion
ChemSusChem ( IF 7.5 ) Pub Date : 2018-10-15 , DOI: 10.1002/cssc.201801486
Qiming Sun ₁ , Ning Wang ₁ , Risheng Bai ₁ , Guangrui Chen ₁ , Zhiqiang Shi ₁ , Yongcun Zou ₁ , Jihong Yu _{1,

2}

Affiliation

Significant interest has emerged in the development of nanometer‐sized and hierarchical silicoaluminophosphate zeolites (SAPO‐34) because of their enhanced accessibility and improved catalytic activity for methanol‐to‐olefin (MTO) conversion. A series of nanometer‐sized SAPO‐34 catalysts with tunable hierarchical structures was synthesized in a Al₂O₃/H₃PO₄/SiO₂/triethylamine(TEA)/H₂O system by using a mesoporogen‐free nanoseed‐assisted method. The nanometer‐sized hierarchical S_H‐3.0 catalyst (TEA/Al₂O₃=3.0) possessed the highest crystallinity, highest abundance of intracrystalline meso‐/macropores, and the most suitable acidity among all obtained catalysts, showing the highest ethylene and propylene selectivity of 85.4 %. This is the highest reported selectivity for MTO reactions under similar conditions. Detailed analysis of the coke produced during the reaction revealed that the small‐sized methyl‐substituted benzene and bulky methyl‐substituted pyrene were mainly located inside the crystals instead of on the surface of the crystals, which provided further insight into understanding the deactivation of the SAPO‐34 catalyst during MTO reaction. Significantly, the simple and cost‐effective synthetic process and superb catalytic performance of the nanometer‐sized hierarchical SAPO‐34 is promising for their practical large‐scale application for MTO conversion.

中文翻译：

低模板消耗和出色的甲醇制烯烃转化率的无介孔原合成SAPO-34分层体系

由于纳米级和分级级硅铝磷酸盐沸石（SAPO-34）的可及性增强，并且甲醇-烯烃（MTO）转化的催化活性得到了提高，因此人们对其开发产生了浓厚的兴趣。通过使用无介孔原的纳米种子辅助方法，在Al ₂ O ₃ / H ₃ PO ₄ / SiO ₂ /三乙胺（TEA）/ H ₂ O体系中合成了一系列具有可调层次结构的纳米级SAPO-34催化剂。。纳米级分级S _H ‐3.0催化剂（TEA / Al ₂ O ₃= 3.0）在所有获得的催化剂中具有最高的结晶度，最高的晶内中/大孔丰度以及最合适的酸度，显示出最高的乙烯和丙烯选择性85.4％。这是在相似条件下对MTO反应的最高选择性报道。对反应过程中产生的焦炭的详细分析表明，小尺寸的甲基取代的苯和大体积的甲基取代的mainly主要位于晶体内部，而不是晶体表面，这为进一步理解该化合物的失活提供了进一步的见识。 MTO反应期间的SAPO-34催化剂。显着地，

更新日期：2018-10-15

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