Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2021-09-16 , DOI: 10.1016/j.micromeso.2021.111410 Mengyue Li 1 , Yi Zhai 1 , Xubin Zhang 1 , Fumin Wang 1 , Guojun Lv 2 , Mengyao Li 1 , Qing Zhang 1 , Yongkui Liu 1
It is of great significance to develop a novel strategy to synthesize hollow zeolite without using mesoporogens due to its extremely short diffusion length. Ferric nitrate as a common iron source and structure direction agent has been used for synthesizing Fe-doped zeolite. However, the effect of ferric nitrate on the morphology of zeolite has not yet been elaborated. Here, we successfully synthesized hollow MFI zeolite with a framework iron-rich surface by using ferric nitrate as an iron source and seed-assistant strategy. It is the first time to propose that inorganic iron has the hollow structure-directing effect. Herein, by comparatively investigated the effect of iron content on the structure and evolution process of hollow zeolite, a novel crystallization mechanism has been proposed based on the competitive relationship between crystallization and dissolution rates. When the Si/Fe ratio reaches 25, the internal dissolution rate of seeds is faster than the surface crystallization rate of zeolite, the hollow structures are acquired. The obtained Fe-doped hollow zeolite exhibits superior catalytic performance for the reaction of phenol degradation. In this reaction, the higher effectiveness factor (η) close to 1 of Fe-doped hollow zeolite confirmed by calculations indicates its superior mass transferability.
中文翻译:
九水硝酸铁诱导合成高骨架铁含量空心沸石
由于空心沸石的扩散长度极短,因此在不使用介孔原的情况下开发一种合成空心沸石的新策略具有重要意义。硝酸铁作为常用的铁源和结构导向剂已被用于合成掺铁沸石。然而,硝酸铁对沸石形态的影响尚未详细阐述。在这里,我们通过使用硝酸铁作为铁源和种子辅助策略,成功合成了具有骨架富铁表面的空心 MFI 沸石。首次提出无机铁具有中空结构导向作用。在此,通过比较研究铁含量对空心沸石结构和演化过程的影响,基于结晶和溶解速率之间的竞争关系,提出了一种新的结晶机制。当Si/Fe比达到25时,晶种的内部溶解速度快于沸石的表面结晶速度,得到空心结构。所获得的Fe掺杂中空沸石对苯酚降解反应具有优异的催化性能。在该反应中,经计算证实,掺杂 Fe 的空心沸石具有较高的接近 1 的效率因子(η),表明其具有优异的传质能力。所获得的Fe掺杂中空沸石对苯酚降解反应具有优异的催化性能。在该反应中,经计算证实,掺杂 Fe 的空心沸石具有较高的接近 1 的效率因子(η),表明其具有优异的传质能力。所获得的Fe掺杂中空沸石对苯酚降解反应具有优异的催化性能。在该反应中,经计算证实,掺杂 Fe 的空心沸石具有较高的接近 1 的效率因子(η),表明其具有优异的传质能力。