Polyoxometalate-based 3DOM ZrO 2 material for deep oxidative desulfurization of DBT with ultrahigh stability
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Polyoxometalate‑based 3DOM ZrO2 material for deep oxidative desulfurization of DBT with ultrahigh stability Yue Du1 · Lina Zhou1 · Zhenhui Liu2 · Lun Yang1
© Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract Highly ordered three-dimensional (3DOM) macroporous polyoxometalate (POM)-based zirconia hybrids with relatively high surface area and interconnected pore structure have been fabricated by colloidal crystal template method. Owing to the evenly distributed POM active sites, large-scaled 3D ordered macroporous structure, and high porosity of as-synthesized POM-based ZrO2 composite, it exhibits excellent extractive-oxidative desulfurization activity and recyclability. 500 ppm of dibenzothiophene (DBT) in the model fuel can be removed within 2 h under mild conditions and no obvious loss of catalytic activity even after 20 times. The oxidative reaction of DBT follows pseudo-first-order kinetics, corresponded to an Arrhenius activation energy of 61.1 kJ/mol. Keywords 3DOM zrO2 · Phosphotungstic acid · Oxidative desulfurization
1 Introduction Nowadays, increasingly stringent emissions and fuel oil standards in the petroleum refining industry have been established to achieve ultra-clean light oil. Currently, hydrodesulfurization (HDS) has been a widely used industrial desulfurization technology in the petroleum refineries which is effective to reduce the contents of aliphatic and acyclic sulfur-containing compounds in fuel oil, including thiols, sulfides, and disulfides [1]. However, the catalytic efficiency of HDS to benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyl dibenzothiophene (4,6-DMDBT) Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10934-020-00969-y) contains supplementary material, which is available to authorized users. * Lina Zhou [email protected] * Zhenhui Liu [email protected] Yue Du duyue‑[email protected] 1
Institute for Advanced Materials, Hubei Normal University, Huangshi 435002, People’s Republic of China
School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, Hubei, People’s Republic of China
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is relatively low, which can be attributed to the high steric resistance of thiophene derivatives. To effectively remove these pertinacious sulfur compounds, alternative non-HDS desulfurization technologies have been extensively investigated, including adsorption desulfurization [2], extraction desulfurization [3], extractive-oxidative desulfurization (EODS) [4] and so on. Among these methods, EODS process is generating a significant amount of interest due to its mild operation conditions and high efficiency, which is regarded as one of the most promising efficient deep desulfurization technology [5]. In recent years, the Keggin-type of heteropolyacid (HPA) attracts more and more attentions as a typical kind of active compound in the ODS process, due to its pseudo-liquid phase behavior and tunable catalytic property process [6]. However, heteropoly acid is high solub
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