Efficient esterification over hierarchical Zr-Beta zeolite synthesized via liquid-state ion-exchange strategy

沸石 硅醇 离子交换 介孔材料 离子 化学 柠檬酸 X射线光电子能谱 路易斯酸 材料科学 选择性 水溶液 酸强度 无机化学 催化作用 核化学 化学工程 有机化学 工程类
作者
Haiwei Li,Shangqing Zhao,Weilong Zhang,Hui Du,Xiaolong Yang,Yanhua Peng,Dezhi Han,Bo Wang,Zhuo Li
出处
期刊:Fuel [Elsevier BV]
卷期号:342: 127786-127786 被引量:44
标识
DOI:10.1016/j.fuel.2023.127786
摘要

The eco-friendly zeolite-based solid acid catalysts constitute an important alternative to the liquid acid catalyst for the production of plasticizer tributyl citrate (TBC), due to their non-corrosive, high hydrothermal stability and easiness to recycle. Herein, a simple acid treatment to the H-Beta zeolite and subsequent incorporation of ZrIV ions into the vacated Al sites were conducted by liquid-state ion-exchange of ZrO(NO3)2 aqueous solution. The ZrIV ions were incorporated into the framework by the expand of the unit cell size, verified by XRD patterns, the emerging new band at ∼198 nm on UV–vis spectra, the enhanced binding energies of the Zr 3d5/2 and Zr 3d3/2 on XPS spectra, as well as the variations of isolated terminal silanol groups (Si-OH) by FTIR and the change of integrated intensity ratio of Q3/Q4 by 29Si MAS NMR. It was illustrated that the Lewis acid sites was the main active sites for esterification reaction and the produced abundant mesopores in the Zr-Beta-x catalysts would facilitate the transportation of TBC. The maximum conversion of citric acid as high as 80 % was obtained on Zr-Beta-128 (SiO2/ZrO2 molar ratio = 128) catalyst with the highest Lewis acid amount. Furthermore, the Zr-Beta-128 zeolite exhibited high stability without any detectable deactivation after 6 cycles with the 100 % selectivity to TBC. The efficient Zr-Beta catalyst could supply a novel possibility for the development of an environmentally-friendly solid acid catalyst with good performance for the TBC production.
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