Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2024-01-29 , DOI: 10.1016/j.micromeso.2024.113028 Yuxin Li , Juanping Zhou , Hu Wen , Haitao Yin , Shunyu Han , Nanzhe Jiang
Clay is a rich aluminosilicate resource with unique advantages as a raw material for zeolites production. However, synthesizing nanosized single-crystalline zeolites through a simple approach using clay remains a significant challenge. In this paper, acid-washed montmorillonite (MSR) was used to prepare nano-H-ZSM-5 single crystals with high crystallinity, uniform grain size and permeable straight pores under the induction of a small amount of organic template tetrapropylammonium hydroxide (TPAOH). Through temperature-staged treatment, the nucleation and growth process of zeolite were decoupled, ultimately achieving precise control over the size of the nano-single crystals. Mechanistic study showed that the low-temperature aging process produces smaller structural units which probably derived from the geopolymer topology of the clay, providing more active sites for zeolite nucleation, leading to the rapid crystallization during the high-temperature process. The porous structure promotes material diffusion, inhibits aromatic cycling and reduces carbon formation in the pores. The large specific surface area and nanoscale multilayer pore structure delay carbon accumulation and increase carbon holding capacity. These properties make nano-ZSM-5 single crystals an excellent choice for high olefin selectivity and long catalytic life in the methanol-to-olefin reaction. This synthetic route provides a general strategy for preparing nanosized zeolite single crystals from clay.
中文翻译:
蒙脱石合成高质量纳米H-ZSM-5单晶沸石及MTO催化研究
粘土是丰富的铝硅酸盐资源,作为沸石生产原料具有独特的优势。然而,使用粘土通过简单的方法合成纳米级单晶沸石仍然是一个重大挑战。本文采用酸洗蒙脱土(MSR)在少量有机模板剂四丙基氢氧化铵(TPAOH)的诱导下制备了结晶度高、晶粒尺寸均匀、具有渗透性直孔的纳米H-ZSM-5单晶。 。通过分级温度处理,将沸石的成核和生长过程解耦,最终实现纳米单晶尺寸的精确控制。机理研究表明,低温老化过程产生更小的结构单元,这可能源自粘土的地质聚合物拓扑,为沸石成核提供更多的活性位点,导致高温过程中的快速结晶。多孔结构促进材料扩散,抑制芳香循环并减少孔中碳的形成。大的比表面积和纳米级多层孔隙结构延缓了碳的积累,提高了持碳能力。这些特性使纳米 ZSM-5 单晶成为甲醇制烯烃反应中高烯烃选择性和长催化寿命的绝佳选择。该合成路线提供了从粘土制备纳米沸石单晶的通用策略。