Aerobic oxidative desulfurization coupling of Co polyanion catalysts and <i>p</i>-TsOH-based deep eutectic solvents through a biomimetic approach

Sun, Lulu; Su, Ting; Xu, Jiajia; Hao, Dongmei; Liao, Weiping; Zhao, Yuchao; Ren, Wanzhong; Deng, Changliang; Lü, Hongying

doi:10.1039/c8gc03941k

Cited by 94 publications

(51 citation statements)

References 52 publications

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“…Various oxidants have been published in the literature, leaving hydrogen peroxide (H 2 O 2 ) as the most frequently used because of its high oxygen density, technical availability, and since water is formed as the only by‐product . Compared to H 2 O 2 , only few publications deal with O 2 or air as oxidant, although it is technically available, low‐cost, and environmentally benign , . The organic sulfur compounds are usually oxidized to their corresponding sulfones or sulfoxides , while increasing their polarity.…”

Section: Introductionmentioning

confidence: 99%

Kinetics of Triphase Extractive Oxidative Desulfurization of Benzothiophene with Molecular Oxygen Catalyzed by HPA‐5

et al. 2020

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The triphasic aerobic extractive desulfurization of benzothiophene (BT) using an aqueous H8[PV5Mo7O40] solution as catalyst and O2 as oxidant was investigated. A time‐resolved analysis of all reaction products in the gas, organic and aqueous phase, is given. The organic sulfur in BT is mainly converted to sulfuric acid. Mass transport limitations can be excluded. The reaction orders are 1 with regard to BT, and 0.5 both for HPA‐5 and O2. Calculated data derived from this mechanism with a power law kinetic approach show good agreement to the experimental data for conversions below 60 %. At higher BT conversions, significant deviations are found, suggesting that acidic products formed in the BT oxidation affect the catalyst and therefore the initial kinetics of the BT oxidation.

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Section: Introductionmentioning

confidence: 99%

Kinetics of Triphase Extractive Oxidative Desulfurization of Benzothiophene with Molecular Oxygen Catalyzed by HPA‐5

et al. 2020

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“…Oxidative desulfurization (ODS) as one of the non‐HDS techniques may be useful for producing clean fuels in limited special situations where it is not necessary to remove nitrogen, oxygen or metal impurities and it is not needed to hydrogenate aromatics and olefins . For this, many research works were focused on the development of active heterogeneous catalysts for ODS of fuel oil .…”

Section: Introductionmentioning

confidence: 99%

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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“…Currently, sulfur‐based compounds have led to serious pollution to the environment . In general, these sulfur‐containing species could be converted into sulfones via oxidation catalysis using suitable catalysts . The POMs‐based inorganic–organic hybrid materials are valuable catalysts for the effective catalytic oxidative desulfurization.…”

Section: Resultsmentioning

confidence: 99%

Highly stable polyoxometalate‐resorcin[4]arene‐based inorganic‐organic complexes for catalytic oxidation desulfurization

Yang

et al. 2019

Applied Organom Chemis

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Self‐assembly of a resorcin[4]arene‐based ligand (TMR4A) with metal salts and H3PMo12O40·xH2O offers two isostructural complexes, namely, [Ni2Cl(TMR4A)2(CH3CN)2]·[PMo12O40]·4CH3CN (1) and [Co2Cl(TMR4A)2(CH3CN)2]·[PMo12O40]·4CH3CN (2). In both 1 and 2, one Cl− anion bridges two metal cations, and each metal cation is further chelated by four 2‐mercaptopyridine N‐oxide groups of one TMR4A, producing a [M2Cl(TMR4A)2]3+ dimer (M = Ni or Co). The negative [PMo12O40]3− as a counter‐anion balances the positive charge. Markedly, 1 and 2 exhibit high stability in aqueous solutions with different pH values and in organic solvents. Remarkably, the efficient heterogeneous catalytic capability for oxidative desulfurization was studied by suing 1 and 2 as recycled catalysts. Moreover, the electrochemical behaviors of the two compounds were discussed as well.

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Aerobic oxidative desulfurization coupling of Co polyanion catalysts and p-TsOH-based deep eutectic solvents through a biomimetic approach

Abstract: The use of coupled catalytic systems with ETMs facilitates the reaction process by transporting electrons from catalysts to the oxidant along a low-energy pathway and, finally, DBT was prone to oxidize to DBTO2.

Cited by 94 publications

References 52 publications

Kinetics of Triphase Extractive Oxidative Desulfurization of Benzothiophene with Molecular Oxygen Catalyzed by HPA‐5

Kinetics of Triphase Extractive Oxidative Desulfurization of Benzothiophene with Molecular Oxygen Catalyzed by HPA‐5

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

Highly stable polyoxometalate‐resorcin[4]arene‐based inorganic‐organic complexes for catalytic oxidation desulfurization

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