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Citric acid and temperature programming assisted synthesized Vanadium Silicate-1 for oxidative desulfurization of dibenzothiophene

Journal 2023 · IF 5.2 · 发表于 2023 年 12 月 4 日
作者: Xiaolu Fan,Fumin Wang,Yi Zhai,Xubin Zhang,Yongwang Li,Kaiwei Wang,Zhibo Xu,Changhao Bing,Jinjin Zhang,Qi Shen,Xinyuan He,Guojun Lv
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摘要

Vanadium-MFI zeolites possess phenomenal potential for catalytic oxidation , while their application is constrained by vanadium content and species distribution. Here, we constructed Vanadium Silicate-1 (VS-1) with enhanced content and preferable distribution by the addition of citric acid in tandem with a temperature-program strategy. Citric acid could modulate the pH in the initial gel and coordinate with vanadium, inhibiting the hydrolysis of vanadium and promoting vanadium incorporation. Moreover, a temperature program was employed to generate unsaturated silicon species, overcoming the tendency of aggregation in vanadium precursor and further promoting vanadium insertion. Furthermore, the effects of the first-stage crystallization temperature and time on the properties of zeolite have been investigated in detail. The sample synthesized through the optimal temperature program achieved 99.9 % dibenzothiophene conversion in 2 h, 10.4 times that of conventional synthesis. To explain the excellent reaction activity, the relationship between different vanadium species and reaction results was investigated. Through linear fitting, V=O(OSi) 2 (OH) was considered as the dominant active species in oxidative desulfurization (ODS) reaction. Notably, the recycled zeolite proved good reusability, further enhancing its promising application prospect.

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