Lin Feng, Ye Zhaoqi, Kong Lingtao, Liu Peng, Zhang Yahong, Zhang Hongbin, Tang Yi
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and Laboratory of Advanced Materials, Fudan University, Shanghai 200433, China.
Institute for Preservation and Conservation of Chinese Ancient Books, Fudan University Library, Fudan University, Shanghai 200433, China.
Nanomaterials (Basel). 2022 May 9;12(9):1601. doi: 10.3390/nano12091601.
The morphology and mesoporosity of zeolite are two vital properties to determine its performance in diverse applications involving adsorption and catalysis; while it remains a big challenge for the synthesis and regulation of zeolites with exceptional morphology/porosity only through inorganic-ions-based modification. Herein, by simply optimizing the alkali metal type (K or Na), as well as alkali/water ratio and crystallization temperature, the zeolite ZSM-5 mesocrystals with diverse mesostructures are simply and controllably prepared via fine-tuning the crystallization mechanism in an organotemplate-free, ions-mediated seed-assisted system. Moreover, the impacts of these key parameters on the evolution of seed crystals, the development and assembly behavior of aluminosilicate species and the solution-phase process during zeolite crystallization are investigated by means of directional etching in NHF or NaOH solutions. Except for the morphology/mesoporosity modulation, their physical and chemical properties, such as particle size, microporosity, Si/Al ratio and acidity, can be well maintained at a similar level. As such, the /-xylene adsorption and catalytic performance of -xylene isomerization are used to exhaustively evaluate the synergistically enhanced catalytic activity and shape selectivity of the obtained products. This work demonstrates the possibility of effectively constructing novel zeolite mesostructures by simply altering parameters on simple ions-controlled crystallization and provides good models to inspect the impacts of mesoporosity or morphology on their catalytic performances.
沸石的形态和介孔性是决定其在吸附和催化等多种应用中性能的两个关键性质;然而,仅通过基于无机离子的改性来合成和调控具有特殊形态/孔隙率的沸石仍然是一个巨大的挑战。在此,通过简单地优化碱金属类型(K或Na)以及碱/水比和结晶温度,在无有机模板、离子介导的晶种辅助体系中,通过微调结晶机制,简单可控地制备了具有不同介观结构的ZSM-5沸石介晶。此外,通过在NHF或NaOH溶液中进行定向蚀刻,研究了这些关键参数对晶种演化、铝硅酸盐物种的生长和组装行为以及沸石结晶过程中溶液相过程的影响。除了形态/介孔率调控外,它们的物理和化学性质,如粒径、微孔率、Si/Al比和酸度,也能很好地保持在相似水平。因此,利用对二甲苯的吸附和对二甲苯异构化的催化性能,全面评估了所得产物协同增强的催化活性和形状选择性。这项工作证明了通过简单改变简单离子控制结晶的参数来有效构建新型沸石介观结构的可能性,并为考察介孔率或形态对其催化性能的影响提供了良好的模型。