A multicomponent assembly approach for the design of deep desulfurization heterogeneous catalysts

Abstract

A multicomponent assembly approach for the design of deep desulfurization heterogeneous catalysts. Dalton Transactions, 45(48), pp. 19511-19518. (doi:10.1039/C6DT03445D) This is the author's final accepted version.There may be differences between this version and the published version. You are advised to consult the publisher's version if you wish to cite from it. Deep desulfurization process is a challenging task and global efforts are focused on the development of new approaches for the reduction of sulfur-containing compounds in fuel oils. In this work, we have proposed a new design strategy for the development of deep desulfurization heterogeneous catalysts. Based on the adopted design strategy, a novel composite material of polyoxometalate (POM)-based ionic liquid-grafted layered double hydroxides (LDHs) was synthesized by an exfoliation/grafting/assembly process. The structural properties of the as-prepared catalyst were characterized using FT-IR, XRD, TG, NMR, XPS, BET, SEM and HRTEM. The heterogeneous catalyst exhibited high activity in deep desulfurization of DBT (dibenzothiophene) 4,6-DMDBT (4,6-dimethyldibenzothiophene) and BT (benzothiophene) at 70 o C in 25, 30 and 40 minutes, respectively. The catalyst can be easily recovered and reused for at least ten times without obvious decrease of its catalytic activity. Such excellent sulfur removal ability as well as the cost efficiency of the novel heterogeneous catalyst can be attributed to the rational design, where the spatial proximity of the substrate and the active sites, the immobilization of ionic liquid onto the LDHs via covalent bonding and the recyclability of the catalyst are carefully considered.

Molybdenum Dioxide in Carbon Nanoreactors as a Catalytic Nanosponge for the Efficient Desulfurization of Liquid Fuels

“…[19] This intermediate is produced when an oxidant, such as hydrogen peroxide, reacts with the Lewis acidic sites of the metal oxide and leads to the formation of electrophilic species, essential to promote efficient ODS. [20][21][22][23] Among catalyst supports, hollow carbon nanostructures, such as carbon nanotubes, may offer several potential benefits for ODS catalysts. Al 2 O 3 , TiO 2 , and SiO 2 supports have recently been shown to improve the performance of ODS catalysts, therefore, selection of an appropriate support is key for refining the oxidative removal of sulfur contaminants in fuel.…”

Recent progress in polyoxometalate-intercalated layered double hydroxides composite materials

“…2008年, Li等 [107] [110] . POM/LDH复合材料兼具有多酸的氧化还原性 和LDH的碱性, 是一类优异的氧化-碱催化双功能催化 图 6 EuW10插层离子液体修饰水滑石作为深度脱硫催化 剂 [109] (网络版彩图) 剂. 在此基础上, Song等 [99] 利用主体层板修饰法制备 了一系列的POM/LDH双功能催化剂Tris-LDH-X(PW9)2 (X=Mn、Fe、Co、Ni、Cu和Zn), 并将它们用于氧化-脑文格碱催化反应中, 显示了优异的催化性能(图7).…”

MoO3 subnanoclusters on ultrasmall mesoporous silica nanoparticles: an efficient catalyst for oxidative desulfurization

“…9,10 Therefore, the ODS has become a promising desulfurization method at present. [11][12][13][14][15][16] However, the catalytic activity of the catalysts now available cannot meet the needs for the industrialization of ODS.…”