Solvent-free methods for the synthesis of ZSM-5 have been previously reported in the literature. These methods typically involve grinding the starting materials together prior to the hydrothermal reaction step. However, very little is known about the reaction intermediates formed during the mechanochemical pre-reaction or about how the pre-reaction impacts the subsequent hydrothermal synthesis conditions (temperature and length of hydrothermal treatment). In this study, the solvent-free synthesis of ZSM-5 was investigated while varying the length and type of grinding (manual, ball-mill) and the components of the reaction mixture. The initial reactions that occurred between the solid-state raw materials during grinding were monitored by powder X-ray diffraction (pXRD). Extended grinding initiates exchange reactions between several reagents to form NaCl and to liberate ammonia and water. The resulting wet paste undergoes facile thermal conversion to crystalline zeolite ZSM-5 framework structures. These results provide valuable insights used to guide the optimization of the synthesis conditions required to prepare stable, crystalline and high surface area ZSM-5 under solvent-free synthesis conditions. The solvent-free approach contributes to the overall goal of a greener, more sustainable ZSM-5 synthesis.

先前已经在文献中报道了用于合成ZSM-5的无溶剂方法。这些方法通常包括在水热反应步骤之前将原料一起研磨。但是，对于在机械化学预反应期间形成的反应中间体或预反应如何影响随后的水热合成条件（水热处理的温度和时间）知之甚少。在这项研究中，研究了ZSM-5的无溶剂合成，同时改变了研磨的长度和类型（手动，球磨）和反应混合物的组成。通过粉末X射线衍射（pXRD）监测在研磨期间固态原料之间发生的初始反应。长时间研磨会引发几种试剂之间的交换反应，从而形成NaCl并释放出氨和水。所得的湿糊剂容易地热转化成结晶沸石ZSM-5骨架结构。这些结果提供了宝贵的见解，可用于指导在无溶剂合成条件下制备稳定，结晶和高表面积的ZSM-5所需的合成条件的优化。无溶剂方法有助于实现更绿色，更可持续的ZSM-5合成的总体目标。无溶剂合成条件下结晶和高表面积的ZSM-5。无溶剂方法有助于实现更绿色，更可持续的ZSM-5合成的总体目标。无溶剂合成条件下结晶和高表面积的ZSM-5。无溶剂方法有助于实现更绿色，更可持续的ZSM-5合成的总体目标。