Nabihan B. Abdul Rahman , Ismaeel Alalq , Matthew J. Wulfers , Dan K. Nielsen , Daniel E. Resasco , Steven P. Crossley
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引用次数: 0
摘要
在酸性沸石上进行芳烃烷基化反应时,最佳催化剂必须表现出对理想产物的形状选择性和对焦炭形成的耐受性,而镧(La)等添加剂可以增强这两方面的性能。本研究探讨了在异丙醇烷基化甲苯的过程中,将 La 加入 H-MOR 及其对形状选择性和催化剂稳定性的影响。La 改变了沸石的孔径和布氏酸度,提高了反应选择性和抗焦性。结果表明,La 通过改变异构体形成过程中的过渡态或限制异构体在沸石通道内的扩散,抑制了体积较大的产物的形成,从而提高了对位选择性,同时抑制了正向选择性。此外,La-MOR 还具有更强的抗焦性,因为 La 促进了焦炭前体向表面碳鎓离子的氢转移,并滴定了布氏酸位点,从而减少了烯烃的低聚作用。这些发现凸显了 La 在调整沸石特性以提高催化性能方面的潜力。
Lanthanum incorporation in H-MOR zeolite to improve shape selectivity and stability against coke formation during the alkylation of toluene with isopropanol
In aromatic alkylation over acidic zeolites, an optimal catalyst must exhibit shape selectivity for desirable products and resistance to coke formation, both of which can be enhanced by additives like lanthanum (La). This study examines the incorporation of La into H-MOR and its effects on shape selectivity and catalyst stability during the alkylation of toluene with isopropanol. La modifies the zeolite’s pore size and Brønsted acidity, improving reaction selectivity and coke resistance. The results show that La enhances para-selectivity while suppressing ortho-selectivity by inhibiting the formation of bulkier products, either by altering transition states in isomer formation or restricting isomer diffusion within the zeolite channels. Additionally, La-MOR demonstrates greater coke resistance, as La promotes hydrogen transfer from coke precursors to surface carbenium ions and titrates Brønsted acid sites, reducing olefin oligomerization. These findings highlight La’s potential for tuning zeolite properties to enhance catalytic performance.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.