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Facile synthesis of ultrafine nanosized ZSM-5 zeolite using a hydroxyl radical initiator for enhanced catalytic performance in the MTG reaction
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-11-28 , DOI: 10.1016/j.micromeso.2020.110780
Chaoqun Feng , Xiaofang Su , Wei Wang , Shutao Xu , Benhan Fan , Qing Xin , Wei Wu

ZSM-5 zeolite is extensively used as a catalyst in the methanol-to-gasoline (MTG) reaction, but many secondary reactions occur because of its large grain size and strong acidity. Thus, it is vital to explore new methods for the preparation of nanosized ZSM-5 zeolite with intercrystalline mesopores to facilitate the diffusion of substances while simultaneously decreasing the acidity. Here, we present a novel procedure for the synthesis of ultrafine nanosized ZSM-5 zeolites (Z5-Sx) at a low temperature (90 °C) that includes the addition of a hydroxyl radical initiator to the initial gel. For comparison, a series of ZSM-5 zeolites (Z5-Ty) were synthesized by crystallization at 170 °C using the traditional hydrothermal method. The influence of hydroxyl radicals on the characteristic properties of the Z5-Sx zeolites was investigated by XRD, SEM, HRTEM, N2 adsorption, and 29Si and 27Al MAS NMR spectroscopy as well as NH3-TPD and Py-IR measurements. The results revealed that the Z5-Sx series samples had smaller crystal sizes and higher mesoporosity than the control samples. In particular, a high content of framework Al atoms was observed at the channel intersections of the Z5-Sx series samples, resulting in a weaker acid strength in comparison with the Z5-Ty samples. This distribution of Al atoms resulted in the excellent catalytic performance of the synthesized Z5-Sx catalysts towards the MTG reaction, and the highest gasoline yield of 65.5% with a methanol conversion of 97.2% was obtained in the reaction with the Z5-S3 catalyst. Markedly, the Z5-S3 sample showed significantly improved catalytic stability and coke tolerance than the control samples.



中文翻译:

使用羟基自由基引发剂轻松合成超细纳米ZSM-5沸石以增强MTG反应中的催化性能

ZSM-5沸石在甲醇制汽油(MTG)反应中被广泛用作催化剂,但由于其较大的粒径和强酸性,会发生许多次要反应。因此,探索具有晶间介孔的纳米级ZSM-5沸石制备新方法以促进物质扩散同时降低酸度至关重要。在这里,我们提出了一种在低温(90°C)下合成超细纳米ZSM-5沸石(Z5-S x)的新方法,该方法包括在初始凝胶中添加羟基自由基引发剂。为了比较,一系列ZSM-5沸石(Z5-T y)是使用传统的水热法在170°C下结晶而合成的。通过XRD,SEM,HRTEM,N 2吸附,29 Si和27 Al MAS NMR光谱以及NH 3 -TPD和Py-IR测量研究了羟基自由基对Z5-S x沸石的特性的影响。。结果表明,与对照样品相比,Z5-S x系列样品具有较小的晶体尺寸和较高的介孔率。尤其是,在Z5-S x系列样品的通道交叉处观察到高含量的骨架Al原子,因此与Z5-T y相比,酸强度较弱样品。Al原子的这种分布导致合成的Z5-S x催化剂对MTG反应具有出色的催化性能,在与Z5-S3催化剂的反应中获得最高的汽油收率65.5%,甲醇转化率为97.2% 。明显地,与对照样品相比,Z5-S3样品显示出显着改善的催化稳定性和焦炭耐受性。

更新日期:2020-12-01
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