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Extractive desulfurization of model fuels with a nitrogen-containing heterocyclic ionic liquid

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1735-1742 doi: 10.1007/s11705-022-2167-x

摘要： A nitrogen-containing ionic liquid was synthesized using an aromatic nitrogen-containing heterocyclic and an amino acid, and applied to the extractive desulfurization process to remove benzothiophene, dibenzothiophene, and 4,6-dimethyldibenzothiphene from a model fuel oil. Chemical characterizations and simulation using Gaussian 09 software confirmed the rationality of an ionic liquid structure. Classification of non-covalent interactions between the ionic liquid and the three sulfur-containing contaminants was studied by reduced density gradient analysis. The viscosity of the ionic liquid was adjusted by addition of polyethylene glycol. Under extraction conditions of the volume of ionic liquid to oil as 1:1 and temperature as room temperature, the desulfurization selectivity of ionic liquid followed the order of 4,6-dimethyldibenzothiphene (15 min) < benzothiophene (15 min) ≈ dibenzothiophene (10 min). Addition of p-xylene and cyclohexene to the fuel oil had little effect. The extractant remained stable and effective after multiple regeneration cycles.

关键词： extractive desulfurization     nitrogen-containing heterocyclic ionic liquid     reduced density gradient analysis     desulfurization selectivity    

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Synthesis and characterization of phosphotungstic acid/activated carbon as a novel ultrasound oxidative desulfurization

Liyan LIU, Yu ZHANG, Wei TAN

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 422-427 doi: 10.1007/s11705-013-1353-2

摘要： Phosphotungstic acid/activated carbon (PTA/AC) catalysts with various AC sizes or PTA content have been synthesized and characterized by N physisorption, X-ray diffraction, Fourier transform infrared spectroscopy and temperature programmed desorption of ammonia. These catalysts were then evaluated in terms of the removal of dibenzothiophene (DBT) by ultrasound-assisted oxidative desulfurization process. The results showed that the DBT conversion obviously increased with the decrease of AC support size and the increase of PTA content. After supporting PTA on AC, the DBT conversion can be improved by 38.9% after ultrasound irradiation for 10 min. In addition, the stability tests of PTA/AC showed that the catalytic oxidative activity of PTA/AC was nearly kept constant after ultrasound irradiation for 20 min, which makes it a promising catalyst to use in ultrasound-assisted oxidative desulfurization process.

关键词： phosphotungstic acid     activated carbon     ultrasound-assisted oxidative desulfurization    

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New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 8-19 doi: 10.1007/s11705-014-1411-4

摘要： Desulfurization of natural gas is achieved commercially by absorption with liquid amine solutions. Adsorption technology could potentially replace the solvent extraction process, particularly for the emerging shale gas wells with production rates that are generally lower than that from the large conventional reservoirs, if a superior adsorbent (sorbent) is developed. In this review, we focus our discussion on three types of sorbents: metal-oxide based sorbents, Cu/Ag-based and other commercial sorbents, and amine-grafted silicas. The advantages and disadvantages of each type are analyzed. Possible approaches for future developments to further improve these sorbents are suggested, particularly for the most promising amine-grafted silicas.

关键词： desulfurization     natural gas desulfurization     hydrogen sulfide sorbent     amine-silica sorbent    

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Deep desulfurization of diesel fuels by catalytic oxidation

YU Guoxian, CHEN Hui, LU Shanxiang, ZHU Zhongnan

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 162-166 doi: 10.1007/s11705-007-0030-8

摘要： Reaction feed was prepared by dissolving dibenzothiophene (DBT), which was selected as a model organosulfur compound in diesel fuels, in -octane. The oxidant was a 30 wt-% aqueous solution of hydrogen peroxide. Catalytic performance of the activated carbons with saturation adsorption of DBT was investigated in the presence of formic acid. In addition, the effects of activated carbon dosage, formic acid concentration, initial concentration of hydrogen peroxide, initial concentration of DBT and reaction temperature on the oxidation of DBT were investigated. Experimental results indicated that performic acid and the hydroxyl radicals produced are coupled to oxidize DBT with a conversion ratio of 100%. Catalytic performance of the combination of activated carbon and formic acid is higher than that of only formic acid. The concentration of formic acid, activated carbon dosage, initial concentration of hydrogen peroxide and reaction temperature affect the oxidative removal of DBT. The higher the initial concentration of DBT in the -octane solution, the more difficult the deep desulfurization by oxidation is.

关键词： organosulfur compound     performic     presence     activated     hydrogen peroxide    

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Catalytic oxidative desulfurization of gasoline using phosphotungstic acid supported on MWW zeolite

Hanlu Wang, Idris Jibrin, Xingye Zeng

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 546-560 doi: 10.1007/s11705-019-1842-z

摘要： Catalysts for the desulfurization of gasoline samples were synthesized via the immobilization of well-dispersed phosphotungstic acid (HPW) on Mobil composition of matter-twenty-two (MWW) zeolite. Characterization results indicated that these catalysts possess a mesoporous structure with the retention of the Keggin structure of immobilized HPW. Relevant reaction parameters influencing sulfur removal were systematically investigated, including HPW loading, catalyst dosage, temperature, initial S-concentration, molar ratio of oxidant to sulfide (O/S), volume ratio of MeCN to model oil (Ext./oil), and sulfide species. The 40 wt-% HPW/MWW catalyst exhibited the highest catalytic activity with 99.6% dibenzothiophene sulfur removal from prepared samples. The 40 wt-% HPW/MWW catalyst was recycled four times and could be easily regenerated. Finally, as an exploratory study, straight-run-gasoline and fluid catalytic cracking gasoline were employed to accurately evaluate the desulfurization performance of 40 wt-% HPW/MWW. Our research provides new insights into the development and application of catalysts for desulfurization of gasoline.

关键词： oxidative desulfurization     phosphotungstic acid     MWW     wet impregnation     adsorption energy    

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Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-021-1397-3

摘要：

• Synthesis of NS-CNTS is used in a high desulfurization performance.

关键词： Dibenzothiophene (DBT)     Tertiary methyl mercaptan     Adsorption     Carbon nano tube (CNT)     Desulfurization     Doping    

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Activity and characteristics of “Oxygen-enriched” highly reactive absorbent for simultaneous flue gas desulfurization

Yi ZHAO,Tianxiang GUO,Zili ZANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 222-229 doi: 10.1007/s11783-014-0636-2

摘要： An “Oxygen-enriched” highly reactive absorbent was prepared by mixing fly ash, lime and a small quantity of KMnO for simultaneous desulfurization and denitrification. Removal of SO and NO simultaneously was carried out using this absorbent in a flue gas circulating fluidized bed (CFB). The highest simultaneous removal efficiency, 94.5% of SO and 64.2% of NO, was achieved under the optimal experiment conditions. Scanning Electron Microscope (SEM) and Accessory X-ray Energy Spectrometer (EDX) were used to observe the surface characteristics of fly ash, lime, “Oxygen-enriched” highly reactive absorbent and the spent absorbent. An ion chromatograph (IC) and chemical analysis methods were used to determine the contents of sulfate, sulfite, nitrate and nitrite in the spent absorbents, the results showed that sulfate and nitrite were the main products for desulfurization and denitrification respectively. The mechanism of removing SO and NO simultaneously was proposed based on the analysis results of SEM, EDX, IC and the chemical analysis methods.

关键词： “Oxygen-enriched” highly reactive absorbent     Surface characteristics     Flue gas circulating fluidized bed     Simultaneous desulfurization and denitrification    

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Enhanced desulfurization performance of hybrid membranes using embedded hierarchical porous SBA-15

Ye Zhang, Jian Song, Josue Quispe Mayta, Fusheng Pan, Xue Gao, Mei Li, Yimeng Song, Meidi Wang, Xingzhong Cao, Zhongyi Jiang

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 661-672 doi: 10.1007/s11705-019-1830-3

摘要： The utilization of materials with a hierarchical porous structure as multi-functional additives is highly attractive in the preparation of hybrid membranes. In this study, novel hybrid membranes are designed by embedding hierarchical porous Santa Barbara Amorphous 15 (SBA-15) with a dual-pore architecture (micropores and mesopores) for pervaporation desulfurization. The SBA-15 with cylindrical mesopores provides molecular transport expressways to ensure improved permeability, while micropores on the wall have molecular sieving effects that are essential for the enhancement of permselectivity of thiophene molecules. Considering thiophene/ -octane mixture as a model system, the hybrid membrane with embedded 6 wt-% SBA-15 exhibits optimal pervaporation desulfurization performance with a permeation flux of 22.07 kg·m ·h and an enrichment factor of 6.76. Moreover, the detailed structure and properties of hybrid membranes are systematically characterized. This study demonstrates the immense potential of hierarchical porous materials as additives in membranes to simultaneously increase permeability and permselectivity.

关键词： hybrid membranes     hierarchical porous SBA-15     sieving effect     pervaporation     desulfurization    

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Oxidative desulfurization of fuels using ionic liquids: A review? ?

Hua Zhao,Gary A. Baker

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 262-279 doi: 10.1007/s11705-015-1528-0

摘要： Extractive oxidation, wherein aromatic sulfur-containing compounds are extracted and subsequently oxidized to their corresponding sulfones, has proven to be one of the most effective desulfurization methods for producing ultra-low sulfur content fuels. As non-volatile and highly designable solvents, ionic liquids (ILs) have attracted considerable attention for the oxidative desulfurization of fuels. In this review, we systematically discuss the utility of ILs in catalytic and extractive oxidation, including their role as extractant, catalyst, or both. We also discuss the challenges facing the use of ILs in this regard, including their relatively high cost and excessive viscosity, as well as their efficiency and stability as catalyst.

关键词： oxidative desulfurization     ionic liquids     extraction     fuels     petroleum     polyoxometalates    

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Desulfurization mechanism of FCC gasoline: A review

Liang ZHAO, Yan CHEN, Jinsen GAO, Yu CHEN,

《化学科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 314-321 doi: 10.1007/s11705-009-0271-9

摘要： This paper reviews the most important developments on the desulfurization mechanism of Fluid Catalytic Cracking (FCC) gasoline. First, the origin of sulfur compounds in FCC gasoline and the current developed desulfurization approaches and technologies are briefly introduced, and then the researches on desulfurization mechanism are summarized from experimental and theoretical perspectives. Further researches on the desulfurization mechanism will lay a foundation for optimizing desulfurization sorbents and technologies.

关键词： Catalytic Cracking     foundation     developed desulfurization     desulfurization mechanism     important    

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Reactive adsorption desulfurization over a Ni/ZnO adsorbent prepared by homogeneous precipitation

Aihua KONG, Yanyu WEI, Yonghong LI

《化学科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 170-176 doi: 10.1007/s11705-013-1322-9

摘要： A high-performance Ni/ZnO adsorbent was prepared by homogeneous precipitation using urea hydrolysis and characterized by N adsorption-desorption, X-ray diffraction (XRD), and scanning electron microscope (SEM). The adsorbent was applied to the deep desulfurization of gasoline and showed a high breakthrough sulfur capacity and a remarkably high volume hourly space velocity. The effects of coexisting olefins in gasoline as well as adsorptive conditions on the adsorptive performance were examined. It was found that olefins in gasoline had a slightly inhibiting effect on the desulfurization performance of the adsorbent. The optimum conditions were 673 K, 1.0 Mpa with a volume hourly space velocity of 60 h . Under the optimum conditions, ultralow sulfur gasoline could be produced and the breakthrough sulfur capacity of the adsorbent was 360 mg-s/g-sorb for the model gasoline.

关键词： nickel     reactive adsorption     desulfurization     thiophene    

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Effect of adjusted mesoscale drag model on flue gas desulfurization in powder-particle spouted beds

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 909-920 doi: 10.1007/s11705-021-2100-8

摘要： An energy minimum multiscale model was adjusted to simulate the mesoscale structure of the flue gas desulfurization process in a powder-particle spouted bed and verified experimentally. The obtained results revealed that the spout morphology simulated by the adjusted mesoscale drag model was unstable and discontinuous bubbling spout unlike the stable continuous spout obtained using the Gidaspow model. In addition, more thorough gas radial mixing was achieved using the adjusted mesoscale drag model. The mass fraction of water in the gas mixture at the outlet determined by the heterogeneous drag model was 1.5 times higher than that obtained by the homogeneous drag model during the simulation of water vaporization. For the desulfurization reaction, the experimental desulfurization efficiency was 75.03%, while the desulfurization efficiencies obtained by the Gidaspow and adjusted mesoscale drag models were 47.63% and 75.08%, respectively, indicating much higher accuracy of the latter technique.

关键词： adjusted mesoscale drag model     particle image velocimetry     water vaporization     desulfurization reaction     numerical simulation    

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Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 203-211 doi: 10.1007/s11705-014-1420-3

摘要： ZSM-5/SBA-15 composite molecular sieves were synthesized using post-synthesis method and characterized by X-ray diffraction and N adsorption-desorption. The oxidative-extration desulfurization of model oil was investigated by using hydrogen peroxide as the oxidant, tetrabutyl ammonium bromide as phase transfer catalyst, dimethyl sulfoxide as extractant, and Zr-ZSM-5/SBA-15, Ag-ZSM-5/SBA-15, Ce-ZSM-5/SBA-15 as catalyst. Under the optimal conditions, the desulfurization rate decreases in the order: Zr-ZSM-5/SBA-15>Ce-ZSM-5/SBA-15>Ag-ZSM-5/SBA-15. The highest desulfurization rate is 84.53% under the catalysis of Zr-ZSM-5/SBA-15. Kinetics analysis shows that the reaction is pseudo-first-order with the activation energy of 44.23 kJ/mol.

关键词： composite molecular sieve     oxidation desulfuration     extraction     kinetic    

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A thermodynamic study of the removal of HCl and H

Joseph LEE, Bo FENG

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 67-83 doi: 10.1007/s11705-011-1162-4

摘要： Advanced integrated-gasification combined-cycle (IGCC) and integrated-gasification fuel cell (IFGC) systems require high-temperature sorbents that are capable of removing hydrogen chloride and hydrogen sulfide from coal derived gases to very low levels. HCl and H S are highly reactive, corrosive, and toxic gases that must be removed to meet stringent environmental regulations, to protect power generation equipment and to control the emissions of contaminants. The thermodynamic behavior of 13 sorbents for the removal of HCl and H S under various conditions including: initial toxic gas concentration (1–10000 ppm), operating pressure (0.1–11 Mpa), temperature (300 K–1500 K), and the presence of H O were investigated. The correlation between HCl and H S was also examined. Thermodynamic calculations were carried out for the reactions of the 13 sorbents using a FactSage 5.2 software package based on free energy minimization. The sorbents, Na CO , NaHCO , K CO , and CaO are capable of completely removing chlorine at high temperatures (up to ~1240 K) and at high pressures. Water vapor did not have any significant effects on the dechlorination capability of the sorbents. Nine of the sorbents namely; Cu O, Na CO , NaHCO , K CO , CaO, ZnO, MnO, FeO, and PbO, were determined to have great potential as desulfurization sorbents. Cu O and ZnO had the best performance in terms of the optimum operating temperature. The addition of water vapor to the reactant gas produces a slightly detrimental effect on most of the sorbents, but FeO exhibited the worst performance with a reduction in the maximum operating temperature of about 428 K. The dechlorination performance of the alkali sorbents was not affected by the presence of H S in the reactions. However, the desulfurization capability of some sorbents was greatly affected by the presence of HCl. Particularly, the performance of Cu O was significantly reduced when HCl was present, but the performance of FeO improved remarkably. The thermodynamic results gathered are valuable for the developments of better sorbents.

关键词： syngas cleaning     sorbent     desulfurization     dechlorination    

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the electronic and geometric structure of VO/BN@TiO heterostructure for efficient aerobic oxidative desulfurization

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 276-287 doi: 10.1007/s11705-022-2242-3

摘要： Particle size governs the electronic and geometric structure of metal nanoparticles (NPs), shaping their catalytic performances in heterogeneous catalysis. However, precisely controlling the size of active metal NPs and thereafter their catalytic activities remain an affordable challenge in ultra-deep oxidative desulfurization (ODS) field. Herein, a series of highly-efficient VOx/boron nitride nanosheets (BNNS)@TiO2 heterostructures, therein, cetyltrimethylammonium bromide cationic surfactants serving as intercalation agent, BNNS and MXene as precursors, with various VOx NP sizes were designed and controllably constructed by a facile intercalation confinement strategy. The properties and structures of the prepared catalysts were systematically characterized by different technical methods, and their catalytic activities were investigated for aerobic ODS of dibenzothiophene (DBT). The results show that the size of VOx NPs and V5+/V4+ play decisive roles in the catalytic aerobic ODS of VOx/BNNS@TiO2 catalysts and that VOx/BNNS@TiO2-2 exhibits the highest ODS activity with 93.7% DBT conversion within 60 min under the reaction temperature of 130 °C and oxygen flow rate of 200 mL·min–1, which is due to its optimal VOx dispersion, excellent reducibility and abundant active species. Therefore, the finding here may contribute to the fundamental understanding of structure-activity in ultra-deep ODS and inspire the advancement of highly-efficient catalyst.

关键词： oxidative desulfurization     boron nitride     vanadium     MXene     intercalation confinement    

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标题 作者 时间 类型 操作

Extractive desulfurization of model fuels with a nitrogen-containing heterocyclic ionic liquid

期刊论文

Synthesis and characterization of phosphotungstic acid/activated carbon as a novel ultrasound oxidative desulfurization

Liyan LIU, Yu ZHANG, Wei TAN

期刊论文

New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

期刊论文

Deep desulfurization of diesel fuels by catalytic oxidation

YU Guoxian, CHEN Hui, LU Shanxiang, ZHU Zhongnan

期刊论文

Catalytic oxidative desulfurization of gasoline using phosphotungstic acid supported on MWW zeolite

Hanlu Wang, Idris Jibrin, Xingye Zeng

期刊论文

Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

期刊论文

Activity and characteristics of “Oxygen-enriched” highly reactive absorbent for simultaneous flue gas desulfurization

Yi ZHAO,Tianxiang GUO,Zili ZANG

期刊论文

Enhanced desulfurization performance of hybrid membranes using embedded hierarchical porous SBA-15

Ye Zhang, Jian Song, Josue Quispe Mayta, Fusheng Pan, Xue Gao, Mei Li, Yimeng Song, Meidi Wang, Xingzhong Cao, Zhongyi Jiang

期刊论文

Oxidative desulfurization of fuels using ionic liquids: A review? ?

Hua Zhao,Gary A. Baker

期刊论文

Desulfurization mechanism of FCC gasoline: A review

Liang ZHAO, Yan CHEN, Jinsen GAO, Yu CHEN,

期刊论文

Reactive adsorption desulfurization over a Ni/ZnO adsorbent prepared by homogeneous precipitation

Aihua KONG, Yanyu WEI, Yonghong LI

期刊论文

Effect of adjusted mesoscale drag model on flue gas desulfurization in powder-particle spouted beds

期刊论文

Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

期刊论文

A thermodynamic study of the removal of HCl and H

Joseph LEE, Bo FENG

期刊论文

the electronic and geometric structure of VO/BN@TiO heterostructure for efficient aerobic oxidative desulfurization

期刊论文