晶种法制备MWW型沸石分子筛用于甲烷脱氢芳构化反应研究OA
Study on MWW-type zeolites prepared by seed-assisted method for methane dehydroaromatization
甲烷脱氢芳构化(MDA)是非石油路线制备芳烃的重要途径,探讨催化剂的孔道结构对其MDA反应催化性能的影响,在指导高性能催化剂的制备上具有重要意义.通过晶种法合成了MWW型沸石分子筛(MCM-56和MCM-22),采用XRD、TEM、SEM和N2吸/脱附对Mo/MCM-56和Mo/MCM-22催化剂的物相、形貌和孔道结构进行了表征分析,并探究了MWW型沸石分子筛中不同孔道体系对Mo/MCM-56和Mo/MCM-22催化剂的MDA反应催化性能的影响.结果表明,晶种法大幅缩短了沸石分子筛的晶化时间,且MWW型沸石分子筛结构与晶种结构密切相关.在相同条件下(700℃、100 kPa)反应9.0 h后,Mo/MCM-22催化剂比Mo/MCM-56催化剂具有更高的芳烃选择性(95%左右)与芳烃产率(7.5%左右)以及更优异的催化稳定性,从而推测Mo/MCM-22催化剂中通过二维MWW沸石纳米片缩合形成的十二元环超笼是MDA反应的主要场所.本研究揭示了MWW型沸石分子筛中不同孔道体系对催化剂的MDA反应催化性能具有重要影响,以期为高产物选择性、高稳定性MDA催化剂的设计提供新思路.
Methane dehydroaromatization(MDA)represents a promising non-petroleum route for aromatic production.Exploring the effects of the pore structures of catalysts on their MDA reaction catalytic performances is crucial for developing high-efficiency catalysts.MWW-type zeolites(MCM-56 and MCM-22)were synthesized by seed-assisted method.The phases,morphologies and pore structures of Mo/MCM-56 and Mo/MCM-22 catalysts were characterized by XRD,TEM,SEM,and N2 adsorption/desorption.Furthermore,the effects of different pore channel systems of MWW-type zeolites on catalytic performances of Mo/MCM-56 and Mo/MCM-22 catalysts for MDA reaction were investigated.The results show that the seed-assisted method significantly reduces crystallization time of zeolites,and the structures of MWW zeolites are closely related to the structures of seeds.After reacting for 9.0 h under the same conditions(700℃,100 kPa),Mo/MCM-22 demonstrates higher aromatic selectivity(around 95%)and aromatic yield(around 7.5%),and superior catalytic stability compared to Mo/MCM-56.Therefore,it is speculated that the 12-membered ring supercages,formed through condensation of adjacent two-dimensional MWW zeolite nanosheets in Mo/MCM-22 catalyst,serves as the primary sites for MDA reaction.The study reveals that different pore channel systems of MWW zeolites have significant effects on the catalytic performance of catalysts for MDA reaction,providing new ideas for designing highly selective and stable MDA catalysts.
李卫强;董新法;樊栓狮;郎雪梅;王燕鸿;钟鎏盈;李刚
华南理工大学 化学与化工学院,广东 广州 510641佛山灿石科技有限公司,广东 佛山 528311华南理工大学 化学与化工学院,广东 广州 510641华南理工大学 化学与化工学院,广东 广州 510641华南理工大学 化学与化工学院,广东 广州 510641华南理工大学 化学与化工学院,广东 广州 510641华南理工大学 化学与化工学院,广东 广州 510641
化学化工
甲烷脱氢芳构化MWW型沸石催化剂晶种法
methane dehydroaromatizationMWW-type zeolitescatalystsseed-assisted method
《低碳化学与化工》 2026 (1)
32-39,62,9
中央高校基本科研业务费专项资金(2024ZYGXZR100).
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