Telles de Souza Julia, Ferreira Young Alexandre, Sousa-Aguiar Eduardo F, Romano Pedro N, García-Martínez Javier, De Almeida João M A R
Escola de Química, Universidade Federal do Rio de Janeiro, Av. Athos da Silveira Ramos, 149, Rio de Janeiro 21941-909, Brazil.
LIPCAT (Laboratório de Intensificação de Processos e Catálise), Universidade Federal do Rio de Janeiro (UFRJ), Rio de Janeiro 21941-594, Brazil.
ACS Catal. 2025 Mar 4;15(6):4586-4595. doi: 10.1021/acscatal.4c07182. eCollection 2025 Mar 21.
This study presents a series of Interzeolite Transformation Intermediates (ITIs) derived from FAU-to-FER interconversion. These hybrid materials, obtained through precise control of the interconversion process, exhibit both large mesoporosity and FER topology-type pore confinement, resulting in high conversion and remarkable shape selectivity despite their disordered structure at the long range. We demonstrated this unique combination of properties in three different catalytic tests. The local order within these ITIs is sufficient to create pore confinement, which not only produces remarkable shape selectivity but also enhances conversion by increasing accessibility. Specifically, the ITIs show a 10-fold increase in activity for Friedel-Crafts alkylation, a 16-fold increase in activity for triisopropylbenzene (TiPBz) cracking, and a two-fold increase in methanol dehydration to dimethyl ether (DME) compared to commercial ferrierite all while maintaining the selectivity of FER. These results highlight the potential of FAU-to-FER ITIs as high-performance catalysts that combine the accessibility of disordered structures with the selectivity typically associated with well-ordered zeolites, opening avenues in zeolite-based catalysis.
本研究展示了一系列由FAU向FER相互转化衍生而来的沸石间转化中间体（ITIs）。这些通过精确控制相互转化过程获得的杂化材料，兼具大介孔性和FER拓扑型孔限域性，尽管其在长程范围内结构无序，但仍具有高转化率和显著的形状选择性。我们在三种不同的催化测试中证明了这种独特的性能组合。这些ITIs内部的局部有序性足以形成孔限域，这不仅产生了显著的形状选择性，还通过增加可及性提高了转化率。具体而言，与商业镁碱沸石相比，ITIs在傅克烷基化反应中的活性提高了10倍，在三异丙基苯（TiPBz）裂解反应中的活性提高了16倍，在甲醇脱水制二甲醚（DME）反应中的活性提高了2倍，同时保持了FER的选择性。这些结果突出了FAU向FER的ITIs作为高性能催化剂的潜力，它将无序结构的可及性与通常与有序沸石相关的选择性相结合，为基于沸石的催化开辟了道路。
