We designed a zeolite stacking structure by using hydraulic pressing and programmed temperature calcination synthesis procedures. ZSM-5 type zeolites with particle sizes of approximately 100 nm, 1 μm and 2 μm were used to synthesize stacking ZSM-5 with a size ranging from 45 to 63 μm. The prepared ZSM-5 zeolite stacking structure was used as a support to deposit palladium. The performance of the palladium/stacking ZSM-5 was investigated on Sonogashira coupling reactions. Stacking samples with micro-sized units (1 μm and 2 μm) showed a 200–300% higher turnover number (TON) than their unit counterparts. However, stacking samples with nano-sized units (100 nm) showed decreased TON conversion compared with that of their unit counterparts, probably due to partial destruction of the nano-sized ZSM-5 structure during the stacking synthesis process at high temperature. The palladium/stacking ZSM-5 (micro-sized units) also showed better conversion on different bromides and alkynes than that of traditional homogenous catalysts. Moreover, the stacking composites showed good durability by recycling 4 runs without losing significant catalytic activity. The design of the stacking MFI structure exhibited improved catalytic activity, sustainability and hierarchical-resemblance properties.

我们通过使用水压和程序设计的温度煅烧合成程序设计了一种沸石堆叠结构。使用粒径大约为100 nm，1μm和2μm的ZSM-5型沸石合成尺寸为45至63μm的堆叠ZSM-5。制备的ZSM-5沸石堆叠结构用作沉积钯的载体。在Sonogashira偶联反应上研究了钯/堆叠ZSM-5的性能。堆叠具有微型单位（1μm和2μm）的样品，其周转率（TON）比同等单位高200-300％。但是，与单位尺寸的样品相比，具有纳米尺寸单位（100 nm）的样品堆叠的TON转化率降低，可能是由于在高温下的堆叠合成过程中纳米级ZSM-5结构的部分破坏。与传统的均相催化剂相比，钯/堆积ZSM-5（微型装置）在不同的溴化物和炔烃上也表现出更好的转化率。此外，堆叠的复合材料通过循环4次试验显示出良好的耐久性，而不会损失明显的催化活性。堆叠式MFI结构的设计显示出改进的催化活性，可持续性和层次相似性。