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学者姓名:马永德
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Abstract :
In the present work, the selective hydrodeoxygenation (HDO) performance of stearic acid over in situ MoS2 catalysts produced from various Mo precursors was evaluated. Notably, the in situ MoS2 catalyst generated from [N-8881](2)MoO4-a Mo-based ionic liquid (IL) with oil-soluble property-achieves up to 99.9% of stearic acid conversion with the HDO product octadecane yield of 97.5% at 300 degrees C, 8 MPa, and 6 h. The activity of [N-8881](2)MoO4 for catalyzing the selective HDO reaction is much better than commercial precursors like Mo(CO)(6) and (NH4)(6)Mo7O24. The in situ MoS2 catalysts were thoroughly characterized and analyzed to elucidate the experimental results. Moreover, the reaction pathway of stearic acid was proposed according to the product distribution, and the relative kinetic parameters were also calculated and discussed. The results indicate that applying Mo-based IL as the precursor to generate in situ MoS2 catalyst for the selective HDO of biolipids is highly interesting and desired.
Keyword :
biodiesel biodiesel biolipid biolipid hydrodeoxygenation hydrodeoxygenation ionic liquid ionic liquid MoS2 catalyst MoS2 catalyst
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GB/T 7714 | Shi, Leilian , Chen, Weihao , Ma, Yongde et al. Mo-based ionic liquid as dispersive precursor for effective hydrodeoxygenation of stearic acid: Mechanism and kinetics [J]. | AICHE JOURNAL , 2025 . |
MLA | Shi, Leilian et al. "Mo-based ionic liquid as dispersive precursor for effective hydrodeoxygenation of stearic acid: Mechanism and kinetics" . | AICHE JOURNAL (2025) . |
APA | Shi, Leilian , Chen, Weihao , Ma, Yongde , Zhang, Hongwei , Cai, Zhenping , Cao, Yanning et al. Mo-based ionic liquid as dispersive precursor for effective hydrodeoxygenation of stearic acid: Mechanism and kinetics . | AICHE JOURNAL , 2025 . |
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Developing catalysts enabling reactive separation is a promising strategy to enhance reaction and separation efficiency of esterification processes. Herein, we designed a class of hybrid catalysts with p-toluenesulfonic acid (PTSA) as main catalyst, and hydrogensulfate ILs as support catalyst and extractant. Using the designed catalysts for methyl esterification of long-chain fatty acids, phase splitting can occur, resulting in ester-rich and catalyst-rich phases. Under optimal conditions, the conversion of palmitic acid (PA) gives methyl palmitate (MP) yield of 98.2 % in 3 hat 348.2 K. The catalysts are also applicable for effective conversion of other long-chain fatty acids and can be facilely recycled through liquid-liquid separation without loss of activity. COSMOtherm and Gaussian calculations were performed to rationalize the reactive separation behavior of the designed catalysts. The kinetic and thermodynamic properties of the esterification reaction were also examined using pseudo-homogeneous (PH) model with non-ideality corrections.
Keyword :
Acidic catalyst Acidic catalyst Biodiesel Biodiesel Esterification Esterification Ionic liquid Ionic liquid Reactive separation Reactive separation
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GB/T 7714 | Wu, Wenquan , Zhang, Jiayin , Ma, Yongde et al. Ionic liquid-based hybrid acidic catalysts enabling phase splitting and reactive separation for methyl esterification of long-chain fatty acids [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 311 . |
MLA | Wu, Wenquan et al. "Ionic liquid-based hybrid acidic catalysts enabling phase splitting and reactive separation for methyl esterification of long-chain fatty acids" . | CHEMICAL ENGINEERING SCIENCE 311 (2025) . |
APA | Wu, Wenquan , Zhang, Jiayin , Ma, Yongde , Zhang, Hongwei , Cai, Zhenping , Cao, Yanning et al. Ionic liquid-based hybrid acidic catalysts enabling phase splitting and reactive separation for methyl esterification of long-chain fatty acids . | CHEMICAL ENGINEERING SCIENCE , 2025 , 311 . |
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There is a particular demand to explore low-volatility and structurally tunable absorbents for efficiency, selectivity and reversibility in capturing H2S. For the first time, the performance of deep eutectic solvents (DESs) composed of 1-ethyl-3-methylimidazolium chloride ([Emim]Cl) and acetamide (AA) were examined as physical absorbents for H2S capture. The physical properties of [Emim]Cl-AA DESs, and solubilities of both H2S and CO2 in them were measured. Relevant experimental results demonstrated that the solubilities of H2S in [Emim]Cl-AA DESs (1.1 mol/kg at 298.2 K and 1.023 bar) significantly exceed those of CO2 (0.040 mol/kg at 298.2 K and 1.027 bar). [Emim]Cl-AA DESs exhibit higher H2S solubilities and superior ideal H2S to CO2 selectivities (e.g., the ideal H2S/CO2 selectivity of [Emim]Cl-AA (1:0.5) is 28.5 at 298.2 K) than those physical absorbents ever reported. The recyclability of [Emim]Cl-AA DESs for H2S selective capture was also evaluated, which was found to be very stable in ten continuous absorption and regeneration cycle experiments. The mechanism of H2S capture by [Emim]Cl-AA DESs was finally illustrated at the molecular level with the support of theoretical calculations. © 2024 Elsevier B.V.
Keyword :
Absorption selectivity Absorption selectivity Deep eutectic solvent Deep eutectic solvent H2S capture H2S capture Physical solvent Physical solvent Theoretical calculation Theoretical calculation
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GB/T 7714 | Zheng, L. , Li, X. , Cao, Y. et al. Efficient, selective and reversible capture of hydrogen sulfide by [Emim]Cl-Acetamide deep eutectic solvents [J]. | Journal of Molecular Liquids , 2024 , 413 . |
MLA | Zheng, L. et al. "Efficient, selective and reversible capture of hydrogen sulfide by [Emim]Cl-Acetamide deep eutectic solvents" . | Journal of Molecular Liquids 413 (2024) . |
APA | Zheng, L. , Li, X. , Cao, Y. , Ma, Y. , Zhang, H. , Cai, Z. et al. Efficient, selective and reversible capture of hydrogen sulfide by [Emim]Cl-Acetamide deep eutectic solvents . | Journal of Molecular Liquids , 2024 , 413 . |
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The design of novel practical catalysts is critical for the blossoming of biodiesel green-energy, in which Mo-based catalysts are of particular interest. In this work, an in-situ synthesis method was proposed to obtain a combo Mo-based ionic liquid and SAPO-11 catalyst. The catalyst presents both highly dispersed MoS2 as hydrodeoxygenation active sites and acidic sites for isomerization. MoS2 with a few fine layers can be identified based on TEM images and the Bronsted acid sites are dominant based on Pyridine-IR analysis. A great performance of MoS2/C(8)min-15 %SA can be obtained under optimized reaction conditions with 100 % conversion of methyl palmitate, 75.0 mol% hydrodeoxygenation to n-C-15-C-16, and 20.5 mol % isomerization to i-C-15-C-16. The structure and activity of the catalyst can be retained at least for 4 cycles. Thin layers and high sulfurization, large amount of Br & oslash;nsted acid sites, and suitable reaction conditions are key points to achieve a significant performance and avoid over cracking and deactivation. On basis of detected intermediates and kinetic data simulations, a complex reaction pathway was proposed and the specific k values for each elementary reaction were provided for the hydrodeoxygenation and isomerization of methyl palmitate.
Keyword :
Biodiesel Biodiesel Hydrodeoxygenation Hydrodeoxygenation Isomerization Isomerization Methyl palmitate Methyl palmitate MoS2 MoS2 SAPO-11 SAPO-11
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GB/T 7714 | Ding, Yongxin , Lin, Jun , Yu, Panjie et al. An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization [J]. | FUEL , 2024 , 362 . |
MLA | Ding, Yongxin et al. "An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization" . | FUEL 362 (2024) . |
APA | Ding, Yongxin , Lin, Jun , Yu, Panjie , Zhang, Hongwei , Ma, Yongde , Cai, Zhenping et al. An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization . | FUEL , 2024 , 362 . |
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The efficient deoxygenation of renewable biolipids into liquid alkanes within the diesel range is a key protocol for producing high-quality biofuels. In this work, the conversion of methyl palmitate and raw palm oil were accomplished utilizing a bifunctional catalyst of Ni catalysts supported on B2O3-ZrO2 under solvent-free conditions. Among various Ni loading ratios investigated, the catalyst featuring a 10 % Ni loading achieved 100 % conversion of methyl palmitate and 84.4 % of liquid yield, with approximately 65 % being C15 alkanes. Additionally, more than 91 % of hydrocarbons were also generated from raw palm oil. These results can be attributed to the synergistic interplay between the acid sites, following B2O3 modification, and the presence of Ni species. Furthermore, the analysis of product distribution, gas product detection and the kinetics calculation strongly supports that the deoxygenation process of methyl palmitate primarily follows the hydrodecarbonylation route, leading to the predominant formation of C15 alkane.
Keyword :
Bifunctional catalyst Bifunctional catalyst Biodiesel Biodiesel Deoxygenation Deoxygenation Liquid alkanes Liquid alkanes Methyl palmitate Methyl palmitate
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GB/T 7714 | Yu, Panjie , Xu, Jing , Liang, Rengan et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst [J]. | FUEL , 2024 , 375 . |
MLA | Yu, Panjie et al. "Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst" . | FUEL 375 (2024) . |
APA | Yu, Panjie , Xu, Jing , Liang, Rengan , Cai, Zhenping , Ma, Yongde , Zhang, Hongwei et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst . | FUEL , 2024 , 375 . |
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There is a particular demand to explore low-volatility and structurally tunable absorbents for efficiency, selectivity and reversibility in capturing H2S. For the first time, the performance of deep eutectic solvents (DESs) composed of 1-ethyl-3-methylimidazolium chloride ([Emim]Cl) and acetamide (AA) were examined as physical absorbents for H2S capture. The physical properties of [Emim]Cl-AA DESs, and solubilities of both H2S and CO2 in them were measured. Relevant experimental results demonstrated that the solubilities of H2S in [Emim]Cl-AA DESs (1.1 mol/kg at 298.2 K and 1.023 bar) significantly exceed those of CO2 (0.040 mol/kg at 298.2 K and 1.027 bar). [Emim]Cl-AA DESs exhibit higher H2S solubilities and superior ideal H2S to CO2 selectivities (e.g., the ideal H2S/CO2 selectivity of [Emim]Cl-AA (1:0.5) is 28.5 at 298.2 K) than those physical absorbents ever reported. The recyclability of [Emim]Cl-AA DESs for H2S selective capture was also evaluated, which was found to be very stable in ten continuous absorption and regeneration cycle experiments. The mechanism of H2S capture by [Emim]Cl-AA DESs was finally illustrated at the molecular level with the support of theoretical calculations.
Keyword :
Absorption selectivity Absorption selectivity Deep eutectic solvent Deep eutectic solvent H2S capture H2S capture Physical solvent Physical solvent Theoretical calculation Theoretical calculation
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GB/T 7714 | Zheng, Lu , Li, Xiong , Cao, Yanning et al. Efficient, selective and reversible capture of hydrogen sulfide by [Emim] Cl-Acetamide deep eutectic solvents [J]. | JOURNAL OF MOLECULAR LIQUIDS , 2024 , 413 . |
MLA | Zheng, Lu et al. "Efficient, selective and reversible capture of hydrogen sulfide by [Emim] Cl-Acetamide deep eutectic solvents" . | JOURNAL OF MOLECULAR LIQUIDS 413 (2024) . |
APA | Zheng, Lu , Li, Xiong , Cao, Yanning , Ma, Yongde , Zhang, Hongwei , Cai, Zhenping et al. Efficient, selective and reversible capture of hydrogen sulfide by [Emim] Cl-Acetamide deep eutectic solvents . | JOURNAL OF MOLECULAR LIQUIDS , 2024 , 413 . |
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The effective separation of ammonia (NH3) has important implication for the conversion improvement and pollution control during the synthesis of NH3. In the present work, a novel kind of non-chloride deep eutectic solvents (DESs) were constructed from dihydroxybenzoic acids (DHBAs) and ethylene glycol (EG). The DHBA + EG DESs exhibit several weak acidic sites and hydrogen-bond sites, thus were proposed for NH3 separation. We found that the amounts of NH3 absorbed by DHBA + EG DESs are quite impressive, particularly at reduced pressures. The capacities can reach 5.64 and 11.69 mol/kg at 0.1 and 1 bar respectively, when the temperature of 298.2 K is considered. Besides, after five absorption-desorption cycles, the DHBA + EG DESs can preserve the excellent NH3 absorption performance. The DHAB + EG DESs can also selectively absorb NH3 from N2 and H2 in the mixed gas. The NH3 absorption mechanism of DHBA + EG DESs was further deeply illustrated by spectro-scopic techniques and theoretical calculations.
Keyword :
Absorption capacity Absorption capacity Chloride free Chloride free Deep eutectic solvent Deep eutectic solvent Gas separation Gas separation Multiple site Multiple site
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GB/T 7714 | Zheng, Lu , Zhang, Xinyue , Li, Qiuke et al. Effective ammonia separation by non-chloride deep eutectic solvents composed of dihydroxybenzoic acids and ethylene glycol through multiple-site interaction [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 309 . |
MLA | Zheng, Lu et al. "Effective ammonia separation by non-chloride deep eutectic solvents composed of dihydroxybenzoic acids and ethylene glycol through multiple-site interaction" . | SEPARATION AND PURIFICATION TECHNOLOGY 309 (2023) . |
APA | Zheng, Lu , Zhang, Xinyue , Li, Qiuke , Ma, Yongde , Cai, Zhenping , Cao, Yanning et al. Effective ammonia separation by non-chloride deep eutectic solvents composed of dihydroxybenzoic acids and ethylene glycol through multiple-site interaction . | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 309 . |
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Solid adsorbents with high NH3 separation performance and good stability are particularly important for industrial applications. In our work, few-layered hexagonal boron nitrides (h-BNs) were synthesized and proposed as a kind of solid adsorbent by utilizing the abundant Lewis acidic B atoms on h-BNs. The synthesized h-BNs were investigated for NH3 separation both experimentally and theoretically. It is found that the NH3 isotherms of h-BNs slightly deviate from the ideal profiles, suggesting that the h-BNs enable moderate interactions with NH3. At the pressure of 0.1 and 1 bar, the h-BNs can adsorb as much as 2.33 and 8.67 mmol/g of NH3, respectively. The h-BNs also demonstrate highly selective adsorption of NH3 from other gases such as N2, H2, and CO2, regardless of calculated ideal selectivities or breakthrough adsorption of mixed gases. The NH3 adsorption of h-BNs can be completely reversed, and the h-BNs also exhibit high oxidative resistance, which is of vital importance for the long-term application in industry. Density functional theory calculations and molecular dynamics simulations were further conducted to rationalize the effective separation of NH3 by h-BNs and disclose the underlying mechanism at the molecular level.
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GB/T 7714 | Zhang, Jiayin , Cao, Yanning , Ding, Fengyun et al. Few-Layered Hexagonal Boron Nitrides as Highly Effective and Stable Solid Adsorbents for Ammonia Separation [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 . |
MLA | Zhang, Jiayin et al. "Few-Layered Hexagonal Boron Nitrides as Highly Effective and Stable Solid Adsorbents for Ammonia Separation" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH (2023) . |
APA | Zhang, Jiayin , Cao, Yanning , Ding, Fengyun , Zheng, Lu , Ma, Yongde , Cai, Zhenping et al. Few-Layered Hexagonal Boron Nitrides as Highly Effective and Stable Solid Adsorbents for Ammonia Separation . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 . |
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Dispersed metal sulfides are promising catalysts for the hydroconversion of biolipids to produce second-generation biodiesel. In this work, oil-soluble Mo-based ionic liquids (ILs) were innovatively utilized as the precursors for in situ generation of MoS2 catalysts for the hydroconversion of biolipids. Taking methyl palmitate as the model compound, the excellent activity of in situ generated MoS2 from ionic liquid Mo-based precursors was obtained. The turnover frequencies (TOFs) reached up to 1.6 x 102 h-1 for methyl palmitate conversion and 83 h-1 for hexadecane (C16) yield at 320 degrees C and 0.5 h (42% conversion) under solvent-dilute conditions. The structures of in situ generated MoS2 catalysts were characterized to pro-vide explanations for the catalytic results. Based on the product distributions, the pathway of methyl palmitate hydroconversion was proposed, and the kinetics of methyl palmitate hydroconversion was analyzed in further detail. Applying the Mo-based ILs in the hydroconversion of methyl palmitate and palm oil under solvent-free condition also granted high conversions of feeds and selectivities of HDO products.(c) 2023 Elsevier Inc. All rights reserved.
Keyword :
Biodiesel Biodiesel Dispersed catalyst Dispersed catalyst Hydrodeoxygenation Hydrodeoxygenation Ionic liquid Ionic liquid Kinetics Kinetics
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GB/T 7714 | Cai, Zhenping , Ding, Yongxin , Zhang, Jiayin et al. In situ generation of dispersed MoS2 catalysts from oil-soluble Mo-based ionic liquids for highly effective biolipids hydrodeoxygenation [J]. | JOURNAL OF CATALYSIS , 2023 , 423 : 50-61 . |
MLA | Cai, Zhenping et al. "In situ generation of dispersed MoS2 catalysts from oil-soluble Mo-based ionic liquids for highly effective biolipids hydrodeoxygenation" . | JOURNAL OF CATALYSIS 423 (2023) : 50-61 . |
APA | Cai, Zhenping , Ding, Yongxin , Zhang, Jiayin , Yu, Panjie , Ma, Yongde , Cao, Yanning et al. In situ generation of dispersed MoS2 catalysts from oil-soluble Mo-based ionic liquids for highly effective biolipids hydrodeoxygenation . | JOURNAL OF CATALYSIS , 2023 , 423 , 50-61 . |
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In this work, an oil-soluble ionic liquid (IL) was combined with mixed metal oxide for in situ generation of bifunctional catalysts for slurry-phase heavy oil hydrocracking. The oil-soluble IL selected was trihexylmethylammonium molybdate ([N-6661](2)MoO4), and the mixed metal oxide selected was SiO2-ZrO2. The performance of using [N-6661](2)MoO4 and SiO2-ZrO2 for slurry-phase hydrocracking was examined systematically. It is found that the addition of SiO2-ZrO2 can significantly improve the conversion of residue to distillate and the gas and coke yields are also improved. The MoS2/SiO2-ZrO2 bifunctional catalysts in situ generated in the reaction system were collected for detailed characterizations. The MoS2 slabs are in a highly dispersed and sulfurized status in the matrix of SiO2-ZrO2, and there are also abundant acidic sites in resultant bifunctional catalysts. The kinetics of slurry-phase hydrocracking was further investigated to disclose the reaction routes for the conversion of residue and the role of adding SiO2-ZrO2 in promoting the hydrocracking reactions.
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GB/T 7714 | Ma, Yongde , Wu, Wenquan , Zhang, Jiayin et al. Slurry-Phase Hydrocracking of Heavy Oil with Bifunctional Catalysts In Situ Generated from Oil-Soluble Ionic Liquid and Mixed Metal Oxide [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 , 62 (38) : 15459-15468 . |
MLA | Ma, Yongde et al. "Slurry-Phase Hydrocracking of Heavy Oil with Bifunctional Catalysts In Situ Generated from Oil-Soluble Ionic Liquid and Mixed Metal Oxide" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 62 . 38 (2023) : 15459-15468 . |
APA | Ma, Yongde , Wu, Wenquan , Zhang, Jiayin , Zhang, Hongwei , Cai, Zhenping , Cao, Yanning et al. Slurry-Phase Hydrocracking of Heavy Oil with Bifunctional Catalysts In Situ Generated from Oil-Soluble Ionic Liquid and Mixed Metal Oxide . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2023 , 62 (38) , 15459-15468 . |
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