Yin Xiaoyan, Liu Ning, Han Muhua, Xu Fan, Jia Yun, Song Feng, Cui Hongyou
School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, China.
School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, China.
Ultrason Sonochem. 2023 Nov;100:106598. doi: 10.1016/j.ultsonch.2023.106598. Epub 2023 Sep 14.
Because of containing the same double 6-ring (D6R) building unit, the pure zeolite CHA with lower framework density (FD = 15.1 T/1000 Å) has been transformed from zeolite T with higher framework density (FD = 16.1 T/1000 Å) through ultrasonic-pretreated hydrothermal synthesis in MOH (KOH and NaOH) solution without adding organic template or seed crystals. Ultrasonic pretreatment facilitates the transformation rate and generates high-quality zeolite CHA. The ultrasound condition should be precisely controlled because that CHA phase is metastable, which is inclined to transform to other more stable phase. The ultrasonic conditions at 313 K and 333 K have been investigated in detail. In KOH solution, the ultrasonic treatment at 313 K can effectively restrain the generation of MER phase, however, it is hard to avoid the existence of MER phase when ultrasound temperature is 333 K. In NaOH solution, the samples with ultrasonic treatment of 313 K show the small particles size of about 1 μm, and the GIS framework topology starts to grow with the ultrasonic treatment of 333 K. The products prepared with the appropriate ultrasonic pretreatment represents smaller particles size, larger mesopore volume and higher CO adsorption capacity than the sample without the ultrasonic pretreatment. The structural evolution of interzeolite transformation has been explored by XRD, FT-IR and SEM observations. With the assistance of ultrasound, the parent zeolite T can quickly decompose into intermediate phase and then regenerate into CHA phase.
由于含有相同的双六元环(D6R)构建单元,具有较低骨架密度(FD = 15.1 T/1000 Å)的纯CHA沸石是通过在MOH(KOH和NaOH)溶液中进行超声预处理水热合成,从具有较高骨架密度(FD = 16.1 T/1000 Å)的T沸石转化而来,无需添加有机模板或晶种。超声预处理提高了转化率并生成了高质量的CHA沸石。由于CHA相是亚稳相,倾向于转变为其他更稳定的相,因此超声条件需要精确控制。已详细研究了313 K和333 K的超声条件。在KOH溶液中,313 K的超声处理可有效抑制MER相的生成,然而,当超声温度为333 K时,很难避免MER相的存在。在NaOH溶液中,313 K超声处理的样品显示粒径约为1μm,而333 K超声处理时GIS骨架拓扑开始生长。与未经超声预处理的样品相比,经过适当超声预处理制备的产物具有更小的粒径、更大的介孔体积和更高的CO吸附容量。通过XRD、FT-IR和SEM观察探索了沸石间转化的结构演变。在超声的辅助下,母体T沸石可快速分解为中间相,然后再生成CHA相。