ACS Omega
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2020
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IF 2.87
Qin Wu,Quan Shi,Jiqing Shang,Min Wang,Hansheng Li,Daxin Shi,Yun Zhao,Qingze Jiao
Surface-active heteropolyacid-based ionic liquids with varying alkyl carbon chains were synthesized, which were subsequently analyzed. The desulfurization of fuels was investigated utilizing various surface-active heteropolyacid-based ionic liquids, and acetonitrile was used as the extractant for the coupling of ODS and EDS. The influences of the alkyl group, surface activity, and hydrophobicity of ionic liquids on sulfur removal were studied. The results suggested that the ionic liquids were stable. Among these ionic liquids, [C4ImBS]3[PW12O40] exhibited the best catalytic performance. Using [C4ImBS]3[PW12O40] as the catalyst, the influences of the catalyst amount, aqueous hydrogen peroxide amount, and reaction temperature on the sulfur removal were explored. Under the optimum conditions, the sulfur removal could achieve 100% efficiency. The recycle experiments also proved that the ionic liquid could be reused.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2016
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IF 1.207
Zhen Song,Dian Yu,Qian Zeng,Jingjing Zhang,Hongye Cheng,Lifang Chen,Zhiwen Qi
When evaluating ionic liquids (ILs) for extractive desulfurization (EDS) of fuel oils, the inevitable presence of water in the system may have a significant and in many cases strongly negative effect. However, few studies have considered this particular issue and a promoted water effect on EDS is scarcely reported. In this work, COSMO-RS was firstly employed to calculate the capacity and selectivity for EDS of various IL/H 2 O mixtures, which cover different IL characters and a wide water concentration range. Experiments were then conducted with a representative IL [C 4 MIM][H 2 PO 4 ], whose stable and even promoted extraction performance with a small amount of water was suggested by COSMO-RS. Through analyses of the desulfurization ratio, the cross-solubility and the water content in the desulfurized fuel, the promoted effect of water within a certain range (< 10 wt%) was experimentally demonstrated. Moreover, such effect of water was explained combining the viscosity, the solvent–solute interactions and the COSMO-RS based analysis.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Chenhua Shu,Hua Cheng,Min Zhao,Dan Luo,Feng Zhu,Haijiao Xie
In this work, three deep eutectic solvents (DESs) triethylamine/formic acid ([Et 3 N/FA]), triethylamine/acetic acid ([Et 3 N/PA]), triethylamine/propionic acid ([Et 3 N/AA]) were synthesized and were used for extractive denitrogenation of model oil. Among them [Et 3 N/PA] exhibited reasonably high extraction efficiency for both indole and quinolone. Structure optimization, electrostatic potential analysis and reduced density gradient analysis were performed to explore the synthesis mechanism of DESs and extractive denitrogenation mechanism by DESs taking [Et 3 N/PA] as a representative. The structure of [Et 3 N/PA] were characterized by FTIR and NMR. Results indicate that both strong hydrogen bond and van der Waals are the major force for DESs synthesis. Both hydrogen bonds and van der Waals are responsible for indole removal, while only van der Waals is responsible for quinolone removal. The effect of factors on extraction efficiency was also investigated and results indicate that [Et 3 N]/[PA] has the advantages of short equilibrium time, ability to deal with fuel oils with a wide range of nitrogen contents, excellent performance near room temperature. The presence of olefins and aromatics in fuel oil has negligible negative influence on the extraction efficiency of indole and quinolone. Furthermore, [Et 3 N/PA] exhibits excellent regeneration performance. Consequently, [Et 3 N/PA] is a promising extractant for fuel oil denitrogenation.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
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2012
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IF 1.088
Xiaochun Chen,Ge Liu,Shan Yuan,Charles Asumana,Wenbo Wang,Guangren Yu
A new class of green solvents, known as ionic liquids (ILs), has recently been the subject of intensive research on the extractive desulfurization of fuel oils because of the limitation of the traditional hydrodesulfurization method in catalytically removing thiophenic sulfur compounds. In this work, four thiazolium-based ILs, that is, 3-butyl-4-methylthiazolium dicyanamide ([BMTH][DCA]), 3-butyl-4-methylthiazolium thiocyanate ([BMTH][SCN]), 3-butyl-4-methylthiazolium hexafluorophosphate ([BMTH][PF6]), and 3-butyl-4-methylthiazolium tetrafluoroborate ([BMTH][BF4]), are synthesized. The extractive capability of these ILs in removing thiophene (TS) and dibenzothiophene (DBT) from model fuel oils is investigated. [BMTH][DCA] and [BMTH][SCN] present better extractive desulfurization capability than [BMTH][BF4] and [BMTH][PF6], which may be ascribed to the additional π−π interaction between –C≡N (in [BMTH][DCA] and [BMTH][SCN]) and thiophenic ring (in TS and DBT); DBT in diesel fuel is more efficiently extracted than TS in gasoline. [BMTH][DCA] offers the best desulfurization results, where 64% and 45% sulfur removal are obtained for DBT and TS, respectively, at IL:oil mass ratio of 1:1, 25°C, 20 min. [BMTH][DCA] is thus selected to systematically investigate the effects of temperature, IL:oil mass ratio, initial sulfur content, multiple-extraction, and IL regeneration on desulfurization. The mutual solubility of [BMTH][DCA] with fuel oil is also determined. It is observed that the desulfurization capability is not too sensitive to temperature and initial sulfur content, which is desired in industrial application; the sulfur contents in gasoline and diesel fuel are reduced from 558 ppm to 20 ppm (after 5 cycles) and from 547 ppm to 8 ppm (after 4 cycles), respectively. This work may show a new option for deep desulfurization of fuel oils.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
·
2024
·
IF 10.1
Fawei Lin,Chujun Luan,Huiyi Mao,Chenxu Zhong,Xinlu Han,Guanyi Chen,Lei Che
The petroleum industry and pyrolysis of organic solid waste produce a large amount of low-grade fuel oil characterized by high proportions of heavy fractions, unsaturated compounds, and oxygen content. Catalytic hydro-pyrolysis is an effective approach to improve the quality with co-production of valuable pyrolysis gases and high-grade pyrolysis oils. However, exploration of available and low-cost hydrogen donors is the determining factor for the feasibility of this technique. Given that NH 3 is the excellent hydrogen carrier and with an active molecular structure, this work innovatively proposed NH 3 assisted catalytic pyrolysis that could significantly promote hydrogenation and cleavage reactions to acquire high-quality products and efficient utilization of NH 3 energy. HZSM-5 with specific modification by desilicication and phosphorus loading was selected as the optimal catalyst. The abundant hierarchical pore structure and weak acidity mainly contributed to the excellent catalytic performance. Specifically, 3 + rings aromatics (≥3 rings) disappeared, long-chain alkanes decreased by 10.45 %, while short-chain alkanes increased from 0 to 42.05 % for HO pyrolysis at 550 °C. The stability and universality of this approach were respectively investigated. Meanwhile, the heat value of pyrolysis gas increased by 3766 times under the optimal condition mainly due to the distinctly high yield of C 2 -C 4 combustible hydrocarbons, ca. 429.22 mL/g-oil. Accordingly, the pyrolysis gas could reach the target of energy self-supply for pyrolysis process by in-situ combustion with the residual NH 3 . Additionally, simulation calculations demonstrated that co-combustion of NH 3 and pyrolysis gases increased the laminar burning velocity and enhanced the combustion efficiency of NH 3 . Approximately 37,675 kJ/kg-oil energy could be produced in gas during NH 3 assisted catalytic pyrolysis to provide sufficient heat in pyrolysis with zero natural gas input. Extremely low production of CO 2 , zero natural gas input, and abundant C 2 -C 4 hydrocarbons jointly promoted the negative carbon effect, ca. 948.65 L CO 2 -eq./kg-oil. This study aims to propose NH 3 as a hydrogen donor so that low-grade fuel oil can be upgraded with energy self-supply.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Peiwen Wu,Xin Song,Linjie Lu,Chang Deng,Hongying Lü,Linlin Chen,Haiyan Ji,Duanjian Tao,Wenshuai Zhu
Hexagonal boron nitride (BN) has gained increasing attention in catalysis, such as in the aerobic oxidative desulfurization (ODS) of fuel oils. Heteroatom doping has found can enhance catalytic performance, but understanding different doping modes remains a challenge for designing active catalysts. This research investigates the effect of various oxygen doping modes on the catalytic performance of BN in aerobic ODS of fuel oils. An oxygen-doped BN (BNO) is achieved through strategic modifications, and the study thoroughly examines the effects of different oxygen-doping modes. Detailed results reveal that lattice oxygen doping enhances catalytic activity, while edge hydroxylation oxygen has a negligible effect. Catalytic experiments show the superior performance of BNO, effectively removing aromatic sulfur compounds, achieving 98.4% sulfur removal, under mild conditions. This comprehensive study provides valuable insights into the effect of oxygen doping on BN catalysts and elucidates the underlying mechanisms governing their enhanced catalytic performance in ODS.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
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2015
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IF 1.587
Teng-Jie Ren,Juan Zhang,Yan-Hui Hu,Jun-Pan Li,Meng-Shuai Liu,Di-Shun Zhao
Several metal-based ionic liquids (ILs) were synthesized and used as extractants for the desulfurization of dibenzothiophene (DBT) in simulated fuel oil. The effects of several anion and metal ions, n (ILs)/ n (metal) as mole ratio, V IL / V oil and extractive times on the removal ratio of DBT were investigated in detail. The results showed that [BMIM]HSO 4 /FeCl 3 (BMIM was short for 1-butyl-3-methyl imidazole) was superior to the other ILs for the extractive desulfurization. A total of 100% of DBT was removed at room temperature in 5 min with V [ BMIM ] HSO 4 / FeCl 3 / V oil = 1 : 1 . The extractive activity of [BMIM]HSO 4 /FeCl 3 IL did not change almost after five runs. Extractive desulfurization of different sulfur compounds and commercial diesel fuel oil were also examined. The removal ratios of the sulfur compounds as the reaction substrates were all over 90% and the sulfur content of commercial diesel oil decreased to 120 ppm from 12,400 ppm.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 3
·617
·
IF 4.6
Peng Zuo,Fuyan Zhao,Fanfan Liu,Jinpei Hei,Guozheng Lv,Xianzong Huang,Jun Zhang,Meng Zhang,Yefeng Liu,Tao Ma
A novel tungsten-based heterojunction nanocomposite material was developed for the efficient oxidative desulfurization (ODS) of fuel oil, enabling the production of low-sulfur fuel and a reduction in harmful SOxemissions. In this material, the WC/W2C heterojunction was uniformly immobilized on a porous nitrogen-doped carbon (NC) matrix structure through facile in situ pyrolysis of polyaniline–phosphotungstic acid (PANI/PTA) precursors. The resultant WC/W2C@NC catalyst demonstrated remarkable desulfurization performance, achieving 100% removal of 4000 ppm dibenzothiophene (DBT) in just 15 min at 60 °C in the presence of 0.03 g of WC/W2C@NC and a H2O2/S molar ratio of 2. This exceptional activity is attributed to the synergistic effects stemming from the accelerated electron transfer by the NC matrix, the intricate porous network, and the abundant WC/W2C heterojunction active sites. Moreover, the in situ formation of NC around WC/W2C mitigated active site leaching, ensuring remarkable stability, with a DBT removal rate of 97.2% maintained even after eight recycling cycles. This work provides a versatile and scalable approach for fabricating tungsten-based heterojunction catalysts and highlights the potential of WC/W2C@NC as a high-performance, durable ODS catalyst, paving the way for further advancements in sustainable desulfurization technologies.
研究领域:
材料科学
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环境科学
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能源工程
✓ 已验证
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2012
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IF 2.237
Hong-Xing Zhang,Jia-Jun Gao,Hong Meng,Ying-zhou Lu,Chun-Xi Li
A novel integrated process is proposed for the catalytic oxidative desulfurization of fuel oil, in which the oxidant H2O2 is in situ generated by oxidizing 2-propanol with oxygen, and its feasibility is evaluated in terms of the S-conversion of 3-methylthiophene (3-MT), benzothiophene (BT), and dibenzothiophene (DBT) in octane under varying conditions. The catalysis of [π-C5H5NC16H33]3[PW4O16] is found to be much superior to H3PW12O40 and [(C4H9)4N]3[PW12O40] due to its good dispersivity in oil and adsorptivity for S-compounds. Some influencing factors for the S-conversion were studied, viz., time, temperature, various S-compounds, and the amount of 2-propanol, initiator, oxygen, and catalyst. All factors that favor the production of the 2-propanol radicals affect the desulfurization rate remarkably. Both BT and DBT can be removed efficiently at mild conditions (1.4 MPa O2, 90 °C) in 6 h with S-conversion above 96%, and the resulting sulfones can be separated via settling or filtration.
研究领域:
化学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 34
·15637-15646
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IF 3.591
Yue Liu,Xia Li,Xin Zhou,Yingna Cui
Although desulfurization of deep eutectic solvents (DESs) can achieve high desulfurization efficiency, as liquids, there are many unnecessary troubles in their industrial application, so the immobilization of deep eutectic solvents is very important. In order to develop a more convenient, effective, and green solid extraction desulfurization technology to remove sulfides in fuel, we solidified deep eutectic solvents onto reduced graphene oxide (rGO) with good chemical stability, large specific surface area, and strong adsorption capacity to prepare deep eutectic solvent/rGO composite materials. The deep eutectic solvent/rGO composite materials were characterized by thermogravimetric analysis (TGA), scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR). Through a large number of comparative experiments, the effect of various factors on the removal rate of sulfides in simulated oil was explored. The desulfurization results show that the prepared (TBAC/2p-TsOH)/rGO composite has the best desulfurization effect. With the initial concentration of 1600 ppm dibenzothiophene deep eutectic solvent simulated oil as the substrate and H2O2 as the oxidant, m((TBAC/2p-TsOH)/rGO) : m(simulated oil) : m(H2O2) = 3 : 10 : 1, after reacting for 40 minutes at 25 °C and 800 rpm, the single desulfurization rate of the composite material can reach 99.19%, achieving the deep desulfurization of fuel oil. Besides, the composite material can be separated and recovered by centrifugation or filtration to be reused, and the desulfurization efficiency is hardly reduced. The high desulfurization rate of DES/rGO is mainly due to the following two reasons. The hydrogen bond between the S atom in the sulfide and the active H in the deep eutectic solvents promotes the removal of the sulfide. The advantages of graphene such as ultra-high specific surface area, better adsorption capacity, and amphiphilic properties enhance the affinity of the simulated oil and the composite material so that the sulfur compounds in the simulated oil are in full contact with the deep eutectic solvents on the composite material, and then the sulfur compounds can be efficient removal.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2023
·
IF 2.6
Wenyang Fan,Chunliang Ge,Delong Ding,Liping Deng,Jun Gao,Dongmei Xu
Separation of sulfides from fuel oil is of great significance for environmental protection. In this paper, the organic solvent (sulfolane) was selected to separate sulfides (thiophene and 2-methylthiophene) from model fuel oil ( n -heptane). The liquid–liquid equilibrium data of the mixtures ( n -heptane + thiophene/2-methylthiophene + sulfolane) were measured at 303.15, 313.15 and 323.15 K under 101.3 kPa. The mass conservation of the experimental data were checked, and the reliability of the tie-lie data were evaluated by the Bachman, Hand and Othmer-Tobias equations. The extraction performance of sulfolane was assessed through the separation factor and partition coefficient, and compared with those for other reported solvents, indicating that sulfolane has better extraction performance for thiophene compared with 2-methylthiophene. Then, the quantum chemical calculation was applied to found the separation mechanism of sulfolane. The analysis of electrostatic potential, interaction energies, and reduced density gradient showed that the main interactions between sulfolane and thiophene (or 2-methylthiophene) were van der Waals and weak hydrogen bond forces. Finally, the non-random two-liquid theory (NRTL) and universal quasi-chemical theory (UNIQUAC) models were applied to fit the tie-line data of the investigated mixtures with the root-mean-square deviation (RMSD) lower than 0.01. The mixed surface analysis method based on Gibbs energy topology is used to verify the binary interaction parameters, which provides basic data for simulating the separation process of sulfide in fuel oil.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Lingchao Xu,Xin An,Junfeng She,Hongping Li,Linhua Zhu,Wenshuai Zhu,Huaming Li,Wei Jiang
Heterogeneous catalysts are usually constructed by immobilizing active species on appropriate supports. However, the dispersibility is difficult to precisely control. In this work, three representative Mo-based MOFs (Mo-MOFs) were constructed by assembling various organic linkers and MoO 3 , where the Mo atoms are homogeneously dispersed due to the coordination. The results illustrated that the obtained Mo-MOF-PI synthesized with 2-propyl imidazole as the ligands exhibited an extremely fast reaction rate, achieving 99.4% sulfur removal of DBT within only 12 min. Compared to other similar catalysts, Mo-MOF-PI showed much higher catalytic activity with a turnover frequency value of 19.2 h −1 . Moreover, it can be reused at least 20 times without a dramatic reduction in catalytic performance. Thus, the as-prepared Mo-MOF catalysts show great potential in large-scale industrial applications.
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）