Zhang Peng, Zhuang Jianguo, Yu Jisheng, Guan Yingjie, Zhu Xuedong, Yang Fan
Engineering Research Center of Large-Scale Reactor Engineering and Technology, East China University of Science & Technology, Ministry of Education, Shanghai 200237, China.
State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Sinopec Shanghai Research Institute of Petrochemical Technology Co., Ltd., Shanghai 201208, China.
Nanomaterials (Basel). 2024 May 5;14(9):802. doi: 10.3390/nano14090802.
A series of quaternary ammonium or phosphonium salts were applied as zeolite growth modifiers in the synthesis of hierarchical ZSM-5 zeolite. The results showed that the use of methyltriphenylphosphonium bromide (MTBBP) could yield nano-sized hierarchical ZSM-5 zeolite with a "rice crust" morphology feature, which demonstrates a better catalytic performance than other disinfect candidates. It was confirmed that the addition of MTBBP did not cause discernable adverse effects on the microstructures or acidities of ZSM-5, but it led to the creation of abundant meso- to marco- pores as a result of aligned tiny particle aggregations. Moreover, the generation of the special morphology was believed to be a result of the coordination and competition between MTBBP and Na cations. The as-synthesized hierarchical zeolite was loaded with Zn and utilized in the propane aromatization reaction, which displayed a prolonged lifetime (1430 min vs. 290 min compared with conventional ZSM-5) and an enhanced total turnover number that is four folds of the traditional one, owing to the attenuated hydride transfer reaction and slow coking rate. This work provides a new method to alter the morphological properties of zeolites with low-cost disinfectants, which is of great potential for industrial applications.
在分级ZSM-5沸石的合成中,一系列季铵盐或鏻盐被用作沸石生长改性剂。结果表明,使用甲基三苯基溴化鏻(MTBBP)可得到具有“稻壳”形态特征的纳米级分级ZSM-5沸石,其催化性能优于其他候选消毒剂。证实添加MTBBP对ZSM-5的微观结构或酸度没有明显的不利影响,但由于微小颗粒排列聚集,导致产生了大量介孔至大孔。此外,这种特殊形态的产生被认为是MTBBP与Na阳离子之间配位和竞争的结果。将合成的分级沸石负载Zn并用于丙烷芳构化反应,由于氢化物转移反应减弱和结焦速率缓慢,其显示出延长的寿命(与传统ZSM-5相比为1430分钟对290分钟)以及总转化数提高四倍,是传统沸石的四倍。这项工作提供了一种用低成本消毒剂改变沸石形态特性的新方法,具有很大的工业应用潜力。