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Effect of framework topology of SAPO catalysts on selectivity and deactivation profile in the methanol-to-olefins reaction

机译:SAPO催化剂框架拓扑结构对甲醇 - 烯烃反应中的选择性和失活谱的影响

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摘要

Catalytic performance in the methanol-to-olefins reaction was studied on four 8-ring silicoaluminophosphate (SAPO) molecular sieves with different framework topologies and cavity-windows of various dimensions: SAPO-35 (LEV), SAPO-56 (AFX), STA-7 (SAV), and SAPO-42 (LTA). The four catalysts were compared with the widely investigated SAPO-34 (CHA) and showed remarkable differences in lifetime and products selectivity. In particular, the STA-7 catalyst gave higher selectivity to C3-C4 olefins, while it had methanol conversion capacity similar to that of a SAPO-34 catalyst with similar crystal size and acidity. Organic species retained in the cavities of partially deactivated catalysts were analyzed at different times on stream. The changes in composition of trapped compounds were correlated with those of the effluent products to elucidate the reaction mechanism and the deactivation pathway. The differences in effluent product distribution and trapped coke species suggest that framework topology has a great influence not only on the stability of the materials but also on the products distribution. (C) 2017 Elsevier Inc. All rights reserved.
机译:在四个8环硅铝磷酸盐(SAPO)分子筛上研究了甲醇 - 烯烃反应中的催化性能,具有不同框架拓扑和各种尺寸的腔窗口:SAPO-35(LEV),SAPO-56(AFX),STA -7(SAV)和SAPO-42(LTA)。将四种催化剂与广泛研究的SAPO-34(CHA)进行比较,并显示出寿命和产品的选择性显着差异。特别地,STA-7催化剂对C3-C4烯烃具有更高的选择性,同时它具有与具有相似晶体尺寸和酸度相似的SAPO-34催化剂的甲醇转化能力。在物流上的不同时间分析保留在部分失活催化剂的空腔中的有机物质。被捕获的化合物的组成的变化与流出物产品的组成相关,以阐明反应机制和失活途径。污水产品分布和被困焦炭物种的差异表明,框架拓扑结构不仅对材料的稳定性产生了很大的影响,而且对产品分布进行了很大影响。 (c)2017年Elsevier Inc.保留所有权利。

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