Liu Zhaohui, Mao Min, Yangcheng Ruixue, Lv Shuang
Institute of Advanced Interdisciplinary Studies, School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China.
Molecules. 2024 Apr 28;29(9):2037. doi: 10.3390/molecules29092037.
Small-pore zeolites catalyze the methanol-to-olefins (MTO) reaction via a dual-cycle mechanism, encompassing both olefin- and aromatic-based cycles. Zeolite topology is crucial in determining both the catalytic pathway and the product selectivity of the MTO reaction. Herein, we investigate the mechanistic influence of MCM-35 zeolite on the MTO process. The structural properties of the as-synthesized MCM-35 catalyst, including its confined cages (6.19 Å), were characterized, confirming them as the catalytic centers. Then, the MTO reactions were systematically performed and investigated over a MCM-35 catalyst. Feeding pure methanol to the reactor yielded minimal MTO activity despite the formation of some aromatic species within the zeolite. The results suggest that the aromatic-based cycle is entirely suppressed in MCM-35, preventing the simultaneous occurrence of the olefin-based cycle. However, cofeeding a small amount of propene in methanol can obviously enhance the methanol conversion under the same studied reaction conditions. Thus, the exclusive operation of the olefin-based cycle in the MTO reaction, independent of the aromatic-based cycle, was demonstrated in MCM-35 zeolite.
小孔沸石通过双循环机制催化甲醇制烯烃(MTO)反应,该机制包括基于烯烃和芳烃的循环。沸石拓扑结构对于确定MTO反应的催化途径和产物选择性至关重要。在此,我们研究了MCM-35沸石对MTO过程的机理影响。对合成后的MCM-35催化剂的结构性质进行了表征,包括其受限笼(6.19 Å),证实它们为催化中心。然后,在MCM-35催化剂上系统地进行并研究了MTO反应。尽管在沸石内形成了一些芳烃物种,但向反应器中加入纯甲醇时,MTO活性极低。结果表明,在MCM-35中基于芳烃的循环被完全抑制,从而阻止了基于烯烃的循环同时发生。然而,在相同的研究反应条件下,在甲醇中共同加入少量丙烯可以明显提高甲醇转化率。因此,在MCM-35沸石中证明了MTO反应中基于烯烃的循环独立于基于芳烃的循环的唯一运行方式。