Hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene over NiMo supported on yolk-shell silica catalysts with adjustable shell thickness and yolk size

Yu, Ke; Kong, Wei­min; Zhang, Zhao; Duan, Aijun; Kong, Lian; Wang, Xilong

doi:10.1016/j.jcat.2022.04.012

Cited by 41 publications

(11 citation statements)

References 65 publications

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“…The cavity size increases with the increasing incubation time. The synthesis mechanism of yolk‐shell structure is that the water tolerance of silicate‐CTAB composites produced by double silicon source (TEOS and BTSE) hydrolysis (TEOS are easier attacked by water molecules than BTSE) [40,41] . Thus, the dark core is derived from the silicate‐CTAB composites (created by BTSE) that are difficult to be attacked by water.…”

Section: Resultsmentioning

confidence: 99%

“…The synthesis mechanism of yolk-shell structure is that the water tolerance of silicate-CTAB composites produced by double silicon source (TEOS and BTSE) hydrolysis (TEOS are easier attacked by water molecules than BTSE). [40,41] Thus, the dark core is derived from the silicate-CTAB composites (created by BTSE) that are difficult to be attacked by water. However, the cavity is originated from the dissolved silicate-CTAB composites (produced by TEOS) which are more unstable and vulnerable under the water attack.…”

Section: Temmentioning

confidence: 99%

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Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Kong

Zhang

et al. 2022

ChemistrySelect

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Novel yolk-shell (YS) mesoporous silica materials with different cavity sizes were successfully synthesized. Aluminium was bridged into the yolk-shell framework of silica by a post synthesis method to improve the acidity of YS, namely Al-YS. The corresponding NiMo/Al-YS catalysts were also fabricated and used in the hydrodesulfurization (HDS) reaction of dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT). The NiMo/Al-YS catalyst with the cavity size of 154 nm (NiMo/Al-YS-154) exhibits the superior conversions of DBT (99.2 %) and 4,6-DMDBT (96.1 %) at 340 °C, 4.0 MPa, 10 h À 1 , highest k HDS (13.4 × 10 À 4 mol gÀ 1 h À 1 for DBT and 8.9 mol g À 1 h À 1 for 4,6-DMDBT) and highest TOF for DBT (3.7 h À 1 ) and 4,6-DMDBT (2.3 h À 1 ) among the investigated catalysts. The appropriate cavity size of NiMo/Al-YS-154 catalyst plays the key role in obtaining its superior HDS catalytic performance. Furthermore, the possible reaction networks of DBT and 4, 6-DMDBT HDS over NiMo/Al-YS-x catalysts were also presented.

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Section: Resultsmentioning

confidence: 99%

Section: Temmentioning

confidence: 99%

Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Kong

Zhang

et al. 2022

ChemistrySelect

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“…In the past few years, sulfoxides (SO x ) originating from combustion of sulfur containing compounds in fossil fuels have caused severe environmental issues, which seriously affect the normal life and health of people. , Accordingly, strict laws and regulations have been issued by governments around the world to the regulate the sulfur contents in diesel . Nowadays, hydrodesulfurization (HDS) is the commercial and widely employed technology in industries to remove and/or convert the sulfur compounds, especially thiophene and mercaptan in the fuel product under both a high operating temperature (∼350 °C) and pressure (∼6 MPa). − However, it requires more stringent conditions to achieve ultra-deep removal of aromatic sulfides [dibenzothiophene (DBT) and its derivatives], which is cost ineffective to the manufacturing enterprise.…”

Section: Introductionmentioning

confidence: 99%

Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization

et al. 2023

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The design and preparation of catalysts with both excellent stability and maximum exposure of catalytic active sites is highly desirable; however, it remains challenging in heterogeneous catalysis. Herein, a entropy-stabilized single-site Mo catalyst via a high-entropy perovskite oxide LaMn 0.2 Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 O 3 (HEPO) with abundant mesoporous structures was initiated by a sacrificial-template strategy. The presence of electrostatic interaction between graphene oxide and metal precursors effectively inhibits the agglomeration of precursor nanoparticles in a high-temperature calcination process, thereby endowing the atomically dispersed Mo 6+ coordinated with four O atoms on the defective sites of HEPO. The unique structure of single-site Mo atoms' random distribution with an atomic scale greatly enriches the oxygen vacancy and increases surface exposure of the catalytic active sites on the Mo/HEPO-SAC catalyst. As a result, the obtained Mo/HEPO-SAC exhibits robust recycling stability and ultra-high oxidation activity (turnover frequency = 3.28 × 10 −2 ) for the catalytic removal of dibenzothiophene (DBT) with air as the oxidant, which represents the top level and is strikingly higher than the state-of-the-art oxidation desulfurization catalysts reported previously under the same or similar reaction conditions. Therefore, the finding here for the first time expands the application of single-atom Mo-supported HEPO materials into the field of ultra-deep oxidative desulfurization.

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“…As the environmental legislation becomes stricter, the amount of sulfur in diesel must be removed to less than 10 ppm. 1 Highly active catalysts for deep hydrodesulfurization (HDS) have drawn considerable interest in the removal of refractory sulfur components, such as 4,6-dimethyldibenzothiophene (4,6-DMDBT). 2 Metal phosphides, especially nickel phosphide (Ni 2 P), are considered as a new family of promising hydrotreating catalysts.…”

Section: Introductionmentioning

confidence: 99%

Efficient Ni₂P/SiO₂ Catalysts with Enhanced Performance for the Hydrogenation of 4,6-Dimethyldibenzothiophene and Phenanthrene

Huang

Sun

Liu

et al. 2023

Ind. Eng. Chem. Res.

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Highly dispersed Ni2P catalysts (Ni2P/SiO2-DPx) were prepared by reducing the passivation-free precursors, which were obtained through the phosphidation of nickel phyllosilicate with sodium hypophosphite. The strong metal–support interaction of nickel phyllosilicate and the mild phosphidation conditions prevented the agglomeration of Ni particles and resulted in a smaller Ni2P particle size. The superior catalytic performance of the as-prepared Ni2P/SiO2-DP catalysts was evaluated in hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene and the hydrogenation of phenanthrene, in comparison with Ni2P/SiO2-IM and CoMoS/γ-Al2O3 prepared from a conventional incipient wetness impregnation method. The passivation-free Ni-P/SiO2-DPx precursors showed great storage stability, and Ni2P/SiO2-DP derived from the stored Ni-P/SiO2-DP precursors exhibited negligible loss of HDS activity. This method provides a potential preparation strategy for the industrial applications of transition metal phosphides without the temperature-programmed reduction and the subsequent passivation process.

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Hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene over NiMo supported on yolk-shell silica catalysts with adjustable shell thickness and yolk size

Cited by 41 publications

References 65 publications

Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization

Efficient Ni₂P/SiO₂ Catalysts with Enhanced Performance for the Hydrogenation of 4,6-Dimethyldibenzothiophene and Phenanthrene

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Hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene over NiMo supported on yolk-shell silica catalysts with adjustable shell thickness and yolk size

Cited by 41 publications

References 65 publications

Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Hydrodesulfurization over NiMo Catalysts Supported on Yolk‐shell Silica Materials with Controllable Cavity Size

Single Mo Atoms Stabilized on High-Entropy Perovskite Oxide: A Frontier for Aerobic Oxidative Desulfurization

Efficient Ni2P/SiO2 Catalysts with Enhanced Performance for the Hydrogenation of 4,6-Dimethyldibenzothiophene and Phenanthrene

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Efficient Ni₂P/SiO₂ Catalysts with Enhanced Performance for the Hydrogenation of 4,6-Dimethyldibenzothiophene and Phenanthrene