Enhanced oxidative desulfurization of liquid model fuel under microwave irradiation over W2N@C catalyst nanoarchitectonics

Bhadra, Biswa Nath; Mondol, Md. Mahmudul Hassan; Jhung, Sung Hwa

doi:10.1016/j.cej.2022.135841

Cited by 20 publications

(5 citation statements)

References 54 publications

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“…Several new mechanisms were proposed to describe the oxidation of S-derivatives to the corresponding sulfones and sulfoxides. 64 Considering literature data and experimental evidence, a mechanism for the DBT oxidation with TBHP catalyzed by SiW 12 @ZSTU-10 was proposed (Figure 7). Initially, there is the reaction between the oxidant and the surface of the nanocomposite, which leads to the oxidation at tungsten centers and ends up with the formation of a metal peroxo species.…”

Section: Resultsmentioning

confidence: 99%

“…As mentioned earlier, the oxidation of sulfur compounds followed pseudo-first-order kinetics, although the real mechanism is far more complicated. Several new mechanisms were proposed to describe the oxidation of S-derivatives to the corresponding sulfones and sulfoxides . Considering literature data and experimental evidence, a mechanism for the DBT oxidation with TBHP catalyzed by SiW 12 @ZSTU-10 was proposed (Figure ).…”

Section: Resultsmentioning

confidence: 99%

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Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Sun,

Abazari,

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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Production of hydrocarbon fuels containing sulfur in ultralow levels is in high demand and requires the development of novel catalytic systems for oxidative desulfurization (ODS). Herein, a new nanocomposite SiW 12 @ZSTU-10 catalyst containing H 4 SiW 12 O 40 (SiW 12 ) encapsulated into a zinc(II) 3D metal−organic framework (MOF) (ZSTU-10) was assembled and characterized. The intricate structure and porosity of ZSTU-10 permit efficient encapsulation of the catalytically active SiW 12 cages. The impact of different experimental parameters on the ODS of model oil containing dibenzothiophene as a typical S-based contaminant was evaluated. The SiW 12 @ZSTU-10 catalyst exhibits remarkable activity with up to 99.8% sulfur removal in 30 min. Kinetic features, trapping tests, and mechanistic studies were also performed. Furthermore, the catalyst offered an outstanding thermal and chemical stability, without apparent leaching and decline in the activity after six cycles. Such an improved catalytic efficiency of SiW 12 @ZSTU-10 can be assigned to (i) size-matched occupation of the ZSTU-10 pores by SiW 12 -active species, (ii) prevention of polyoxometalate (POM) leaching from the MOF matrix, (iii) facilitation of the access of S-based substrates to the active sites of SiW 12 , and (iv) excellent stability and recyclability of the obtained nanocomposite. The preset work widens a family of promising nanocomposite catalysts for improving the desulfurization performance of hybrid POM-MOF catalytic systems.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Sun,

Abazari,

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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“…8,12−14 Among them, the hydroxyl radical ( • OH, Φ: 2.8 V) and the superoxide radical ( • O 2 − , Φ: 2.4 V) feature a superior oxidizing ability; 15 thus, ODS reaction kinetics can be significantly improved by inducing the selective generation of radicals. 16,17 However, radicals are competitively consumed by interfering components in complicated real fuels due to their high redox potentials, consequently leading to significant oxidant depletion and fuel quality degradation. 18,19 Therefore, there seems to be a so-called activity-selectivity trade-off in ODS, which impedes further improvements in this technology.…”

Section: ■ Introductionmentioning

confidence: 99%

Electron Delocalization Disentangles Activity-Selectivity Trade-Off of Transition Metal Phosphide Catalysts in Oxidative Desulfurization

Zou,

Wu,

Lin

et al. 2024

Environ. Sci. Technol.

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Breaking the activity-selectivity trade-off has been a long-standing challenge in catalysis. Here, we proposed a nanoheterostructure engineering strategy to overcome the trade-off in metal phosphide catalysts for the oxidative desulfurization (ODS) of fuels. Experimental and theoretical results demonstrated that electron delocalization was the key driver to simultaneously achieve high activity and high selectivity for the molybdenum phosphide (MoP)/tungsten phosphide (WP) nanoheterostructure catalyst. The electron delocalization not only promoted the catalytic pathway transition from predominant radicals to singlet oxygens in H 2 O 2 activation but also simultaneously optimized the adsorption of reactants and intermediates on Mo and W sites. The presence of such dual-enhanced active sites ideally compensated for the loss of activity due to the nonradical catalytic pathway, consequently disentangling the activity-selectivity trade-off. The resulting catalyst (MoWP 2 /C) unprecedentedly achieved 100% removal of thiophenic compounds from real diesel at an initial concentration of 2676 ppm of sulfur with a high turnover frequency (TOF) of 105.4 h −1 and a minimal O/S ratio of 4. This work provides fundamental insight into the structure−activity-selectivity relationships of heterogeneous catalysts and may inspire the development of high-performance catalysts for ODS and other catalytic fields.

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“…Designing an efficacious catalyst/adsorbent is regarded as the key challenge in the desulfurization and denitrogenation processes of fuel oils. So far, many catalysts/adsorbents like Mo, Ti, Cu, W, V, nanocomposites of polyoxometalates, tungsten nitrides, boron nitrides (BNs), WO x -supported ZrO 2 , monoclinic VO 2 , V 2 O 5 /Al 2 O 3 , Co nanoparticles/porous carbon, perovskite, transition metal dichalcogenides, graphene oxide, Bi 3+ -containing compounds, and TBAPW 11 Zn@TiO 2 @PAni have been well documented . However, these materials face challenges of high cost, complicated preparation strategies, compromised performance, and low recyclability.…”

Section: Introductionmentioning

confidence: 99%

Perspectives on Advances in the Catalytic Desulfurization and Denitrogenation of Transportation Fuel Oils Using Graphitic Carbon Nitride and Boron Nitride

et al. 2022

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Expulsion of sulfur-containing compounds as well as nitrogen-containing compounds present in fuel oils is critical because it can cause numerous environmental problems and catalyst deactivation. Because of the limitations of the other catalysts and adsorbents used for desulfurization, a new type of carbon material, i.e., graphitic carbon nitride (g-C3N4), has emerged. It is similar in morphology to graphene having a two-dimensional structure and possessing a band gap of 2.7 eV and is an attractive catalyst attributed to its intriguing characteristics like high intrinsic photoresponsiveness and photoabsorption, semiconductive properties, and better stability. An ample amount of literature has been documented on g-C3N4 applied for the desulfurization and denitrogenation of fuel oils. Due to the analogy of boron with carbon materials, boron nitrides (BN) are also important. In materials chemistry, hexagonal BN (h-BN), often termed as “white graphene”, among the different phases of BN, is highly regarded due to adaptation of diverse morphologies such as nanotubes and nanosheets. BN has been recommended as an emerging and efficacious 2D material in catalysis because it possesses oxidative resistance, chemically inertness, a sp2-bonded layered structure, wide band gap, and higher thermal stability and conductivity. This review systematically encompasses the important reports documented on the applications of g-C3N4 and BNs in fuel oil processing including the synthesis, various properties, and fascinating experimental findings. Later on, key suggestions are put forward for future research directions and new technologies applying g-C3N4 and BN for the processing of transportation fuels. This review could act as a concentrated platform, as a quick access source and great degree of convenience, giving time effective routes for researchers to reported results and designs of novel and efficacious catalysts for the commercialization of desulfurization and denitrogenation technologies.

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Enhanced oxidative desulfurization of liquid model fuel under microwave irradiation over W2N@C catalyst nanoarchitectonics

Cited by 20 publications

References 54 publications

Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Electron Delocalization Disentangles Activity-Selectivity Trade-Off of Transition Metal Phosphide Catalysts in Oxidative Desulfurization

Perspectives on Advances in the Catalytic Desulfurization and Denitrogenation of Transportation Fuel Oils Using Graphitic Carbon Nitride and Boron Nitride

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Enhanced oxidative desulfurization of liquid model fuel under microwave irradiation over W2N@C catalyst nanoarchitectonics

Cited by 20 publications

References 54 publications

Encapsulation of H4SiW12O40 into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Encapsulation of H4SiW12O40 into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Electron Delocalization Disentangles Activity-Selectivity Trade-Off of Transition Metal Phosphide Catalysts in Oxidative Desulfurization

Perspectives on Advances in the Catalytic Desulfurization and Denitrogenation of Transportation Fuel Oils Using Graphitic Carbon Nitride and Boron Nitride

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Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel

Encapsulation of H₄SiW₁₂O₄₀ into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel