Molybdenum-containing dendritic mesoporous silica spheres for fast oxidative desulfurization in fuel

Zhang, Ming; Liu, Jiaqi; Yang, Jiapeng; Chen, Xiao; Wang, Miao; Li, Hongping; Zhu, Wenshuai; Li, Huaming

doi:10.1039/c8qi00987b

Cited by 29 publications

(24 citation statements)

References 62 publications

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“…This means that 4,6‐DMDBT should be easily oxidized when compared with BT and DBT. In fact, some earlier reports displayed the difficulty of oxidation in the order of BT > DBT > 4,6‐DMDBT . However, in this work, the catalytic data show that the conversion of sulfur compounds follows the order of DBT > BT > 4,6‐DMDBT.…”

Section: Resultscontrasting

confidence: 54%

Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil

et al. 2020

ChemistrySelect

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MOF‐808(Zr) as an important member of metal‐organic frameworks (MOFs) has attracted much attention due to its good stability, large surface area and rich zirconium metal centers. However, Zr sites in the structure of MOF‐808(Zr) are inactive in many catalytic reactions due to they are well coordinated with organic ligands like 1,3,5‐benzenetricarboxylic acid (BTC) and formate anions. Thus, removing formate anions have been attempted to create more active sites in the structure for many reactions while maintaining the structural stability. In this work, we report that the formate ligands in MOF‐808(Zr) can be facilely removed by the treatment in hot ethanol for 4 h. The obtained material as a heterogeneous catalyst exhibited superior catalytic activity in the oxidative desulfurization (ODS) reaction of dibenzothiophene (DBT) compared with reported MOFs catalysts. The conversion of DBT in model diesel oil could reach >99 % within a reaction time of 20 min at 323 K, which is five times as that over parent MOF‐808(Zr). As a result, the sulfur content was decreased from 1000 ppm to less than 10 ppm. Such catalytic performance should be mainly attributed to the creation of more active sites in the structure of MOF‐808(Zr) after the removal of formate anions.

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Section: Resultscontrasting

confidence: 54%

Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil

et al. 2020

ChemistrySelect

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“…Specially designed dendritic mesoporous silica nanospheres with center-radial oriented large mesopores were reported earlier by Zhao et al as potential carriers or substrates for development of new functional materials [ 89 , 90 ]. Interestingly, Zhang et al took advantage of the above materials to design a molybdenum-embedded dendritic mesoporous silica sphere using Stöber approach [ 91 ]. As shown in Figure 2 , they introduced active molybdenum species with a concomitant use of ionic liquid (IL) as a metal source into the mesopores of dendritic silica spheres (DSSs).…”

Section: Mesoporous Silica and Mesoporous Silica Nanoparticles In mentioning

confidence: 99%

Section: Mesoporous Silica and Mesoporous Silica Nanoparticles In mentioning

confidence: 99%

“… Schematic representation of dendritic mesoporous Mo-SiO 2 catalyst and its desulfurization mechanism [ 91 ]. …”

Section: Figures Scheme and Tablementioning

confidence: 99%

“…Under optimal conditions, elimination of 4,6-DMDBT could reach 100% in 40 min, and a low dosage of oxidant was required. The recycling performance of the DSS revealed that they could be reused nine times without an appreciable decrease in catalytic activity [91]. Exemplary performance of monolacunary [PW 11 O 39 ] 7-Keggin polyoxometalates in oxidative reactions [92][93][94][95][96] has inspired a few researchers to explore their performance in ODS process, too [97][98][99].…”

Section: Redox Active Msnsmentioning

confidence: 99%

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Recent Advances in Functionalized Mesoporous Silica Frameworks for Efficient Desulfurization of Fuels

Mendiratta

Ali

2020

Nanomaterials

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Considerable health and climate benefits arising from the use of low-sulfur fuels has propelled the research on desulfurization of fossil fuels. Ideal fuels are urgently needed and are expected to be ultra-low in sulfur (10–15 ppm), with no greater than 50 ppm sulfur content. Although several sulfur removal techniques are available in refineries and petrochemical units, their high operational costs, complex operational needs, low efficiencies, and higher environmental risks render them unviable and challenging to implement. In recent years, mesoporous silica-based materials have emerged as promising desulfurizing agents, owing to their high porosity, high surface area, and easier functionalization compared to conventional materials. In this review, we report on recent progress in the synthesis and chemistry of new functionalized mesoporous silica materials aiming to lower the sulfur content of fuels. Additionally, we discuss the role of special active sites in these sorbent materials and investigate the formulations capable of encapsulating and trapping the sulfur-based molecules, which are challenging to remove due to their complexity, for example the species present in JP-8 jet fuels.

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Boron and Nitride Dual vacancies on Metal‐Free Oxygen Doping Boron Nitride as Initiating Sites for Deep Aerobic Oxidative Desulfurization

Dai

Wei

et al. 2020

ChemCatChem

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Boron nitride (BN) is a two‐dimensional ceramic material that has been widely applied in various catalysis reactions. However, endowing the BN material with adequate reactive centers remains to be a considerable challenge. Herein, we propose a tunable boron and nitride dual vacancies strategy to generate highly active oxygen‐doping BN (BNO) material via heat treatment in vacuum. Experimental results indicate that the vacuum treatment fabricates boron and nitride dual vacancies on the BNO. The as‐prepared vacuum treated BNO (V‐BNO) was applied as the initiator to accelerate the aerobic oxidative desulfurization (ODS) of fuel. The boosted aerobic ODS system achieves 100 % sulfur removal in 6 h, and it can be recycled 6 times without any significant performance loss. Meanwhile, the density functional theory (DFT) reveals the reaction pathway on the V‐BNO, ensuring the contribution of boron and nitride dual vacancies to the initiation of the reaction. This work highlights the vital role of dual vacancies as initiating sites for the enhanced aerobic ODS.

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Molybdenum-containing dendritic mesoporous silica spheres for fast oxidative desulfurization in fuel

Abstract: 4,6-DMDBT is absorbed by dendritic mesoporous Mo-SiO2 and then oxidized to 4,6-DMDBTO2 in the presence of TBHP.

Cited by 29 publications

References 62 publications

Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil

Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil

Recent Advances in Functionalized Mesoporous Silica Frameworks for Efficient Desulfurization of Fuels

Boron and Nitride Dual vacancies on Metal‐Free Oxygen Doping Boron Nitride as Initiating Sites for Deep Aerobic Oxidative Desulfurization

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