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Sequential Microwave-Assisted Dealumination and Hydrothermal Alkaline Treatments of Y Zeolite for Preparing Hierarchical Mesoporous Zeolite Catalysts
Topics in Catalysis ( IF 3.6 ) Pub Date : 2020-05-10 , DOI: 10.1007/s11244-020-01268-1
Ringxin Zhang , Duaa Raja , Yong Zhang , Ying Yan , Arthur A. Garforth , Yilai Jiao , Xiaolei Fan

A novel post-synthetic method combining the microwave (MW)-assisted dealumination and hydrothermal (HT) alkaline treatment for obtaining mesoporous Y zeolite catalysts is presented. In the first-step MW-assisted dealumination of the pristine Y zeolite, both the mineral acid (i.e. hydrochloric acid, HCl) and organic carboxylic acids (e.g. oxalic and diethylenetriaminepentaacetic acid) were used (all at 0.16 M), and their effects on the physical and chemical properties of the resulting modified zeolites (after the identical HT alkaline treatment using 0.2 M sodium hydroxide solution) are studied in detail by comprehensive characterisation of the bulk silicon-to-aluminium (SAR) ratio, crystallinity and textural properties. The findings show that, in the developed sequential method, (i) HCl was only effective to achieve the hydrolysis of the zeolite, (ii) carboxylic acids with the function of chelation was very capable of extracting Al species and creating mesopores, and (iii) the mesopores formation is a function of the number of coordination sites in the carboxylic acid. The hierarchical feature of the mesopores in the modified zeolites (using carboxylic acids) was probed by the model reaction of aldol condensation of 1-heptanal with benzaldehyde for the selective formation of jasminaldehyde. The normalised selectivity to jasminaldehyde (with respect to the strong acidity) was proportionally related to the specific mesopores volume of the zeolites, revealing hierarchical porous networks in the relevant modified Y zeolites and indicating the effect of hierarchical mesopores in the zeolites on their catalytic performance.



中文翻译:

Y沸石的连续微波辅助脱铝和水热碱处理,以制备多级介孔沸石催化剂

提出了一种结合微波辅助脱铝和水热碱处理的新型后合成方法,以得到介孔Y型沸石催化剂。在第一步MW辅助的原始Y沸石的铝脱铝中,使用了无机酸(例如盐酸,HCl)和有机羧酸(例如草酸和二亚乙基三胺五乙酸)(均在0.16 M下),通过对整体硅铝比(SAR),结晶度和质构特性进行综合表征,详细研究了所得改性沸石的物理和化学性质(在使用0.2 M氢氧化钠溶液进行相同的HT碱处理后)。研究结果表明,在已开发的顺序方法中,(i)HCl仅有效地实现了沸石的水解,(ii)具有螯合功能的羧酸非常有能力提取Al物种并产生中孔,并且(iii)中孔的形成是羧酸中配位点数量的函数。通过1-庚醛醛缩合与苯甲醛的醛醇缩合反应的模型反应,探讨了改性沸石(使用羧酸)中介孔的层级特征。茉莉醛的标准化选择性(相对于强酸度)与沸石的特定中孔体积成比例相关,揭示了相关改性Y沸石中的分层多孔网络,并表明了沸石中分层中孔对其催化性能的影响。

更新日期:2020-05-10
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