Surface modification of H-ZSM-5 with organo-disilane compound for propylene production from dimethyl ether
Surface modification of H-ZSM-5 with organo-disilane compound for propylene production from dimethyl ether
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DOI：
10.1016/j.micromeso.2019.02.005
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发表时间：
2019-05
影响因子：
5.2
通讯作者：
M. Fujiwara;N. Mimura;O. Sato;A. Yamaguchi
中科院分区：
文献类型：
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作者：
M. Fujiwara;N. Mimura;O. Sato;A. Yamaguchi
对沸石进行有效改性以提高其催化性能是微孔材料化学的一个重要课题。H-ZSM-5型沸石是生产丙烯的强力催化剂，是多种化工产品的重要起始原料，主要来源于化石资源。近年来，由于化石燃料的枯竭风险和全球变暖问题，人们希望利用非化石碳资源生产丙烯。以酸性催化剂为催化剂，积极研究了二甲醚（DME）转化丙烯作为丙烯的替代合成路线。本文报道了用表面改性有机二硅烷化合物1,4-双（羟基二甲基硅基）苯的H-ZSM-5催化剂催化二甲醚制丙烯的研究。用二硅烷化合物表面改性的H-ZSM-5催化剂制备二甲醚丙烯的产率高于未改性的H-ZSM-5催化剂。在480 °C的气流处理下，改性H-ZSM-5有效地再生了反应过程中因形成焦炭而失活的催化剂，再生后的催化剂的丙烯生产活性与失活前的催化剂几乎相当。覆盖在H-ZSM-5外表面的二硅烷化合物的苯环形成的多环芳香族化合物控制了催化活性，提高了丙烯的收率。
The efficient modification of zeolites for improving their catalytic properties is a significant subject of microporous materials chemistry. H-ZSM-5 zeolite is a potent catalyst of the production of propylene as an important start material of a variety of chemical products, which is mainly obtained from fossil resources. Recently, the production of propylene using non-fossil carbon resources are desired because of the depletion risk of fossil fuels and global warming problem. Dimethyl ether (DME) conversion to propylene is actively studied using acid catalysts as an alternative synthetic route of propylene. This paper reports the propylene production from DME using H-ZSM-5 catalyst whose surface was modified with an organo-disilane compound, 1,4-bis(hydroxydimethylsilyl)benzene. An H-ZSM-5 catalyst surfacely modified with the disilane compound produced propylene from DME in higher yield than original (non-modified) H-ZSM-5. Air flow treatment at 480 °C effectively regenerated the modified H-ZSM-5 that was deactivated by coke formation during the reaction, and this regenerated catalyst had a nearly equivalent activity of the propylene production to the catalyst before deactivation. The polycyclic aromatic compounds formed from the benzene ring of the disilane compound that covered the exterior surface of H-ZSM-5 controlled the catalytic activity to increase the yield of propylene.