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1.华南理工大学 化学与化工学院,广东 广州 510641
2.佛山灿石科技有限公司,广东 佛山 528311
李卫强(2000—),硕士研究生,研究方向为分子筛的合成,E-mail:Lwq228617@163.com。
李刚(1983—),博士,教授,研究方向为分子筛的合成与应用,E-mail:fegli@scut.edu.cn。
收稿:2025-06-17,
修回:2025-07-23,
纸质出版:2026-01-25
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李卫强,董新法,樊栓狮等.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[J].低碳化学与化工,2026,51(1):32-39.
LI Weiqiang,DONG Xinfa,FAN Shuanshi,et al.Study on MWW-type zeolites prepared by seed-assisted method for methane dehydroaromatization[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(1):32-39.
李卫强,董新法,樊栓狮等.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[J].低碳化学与化工,2026,51(1):32-39. DOI: 10.12434/j.issn.2097-2547.20250277.
LI Weiqiang,DONG Xinfa,FAN Shuanshi,et al.Study on MWW-type zeolites prepared by seed-assisted method for methane dehydroaromatization[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(1):32-39. DOI: 10.12434/j.issn.2097-2547.20250277.
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N
2
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 N
2
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 °C
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 channe
l 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.
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