Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Tuo Zheng,Haiyan Fan,Jia Zhao,Jile Fu,Songshou Ye,Sajid Ali,Nuowei Zhang,Jinbao Zheng,Binghui Chen
In diesel adsorption desulfurization, the coordination bonding between the adsorbent and sulfur compounds is interfered by aromatic compounds in diesel. Transition metal cation exchanged zeolites Y has exhibits exceptional anti-interference performance. In this work, the influence of electron configuration on coordination bonding is explored, specifically between the adsorbent and substrate, using both experimental and DFT theoretical methods. Initially, NiY, CuY and ZnY were synthesized and evaluated for their desulfurization performance in model solution (sulfur content: 25 ppmw dibenzothiophene [DBT]) with two toluene concentrations (1 w% and 3 w%). It is found that CuY showed the highest performance with retention rate at 70.2 %. Subsequently, DFT calculations revealed the binding energy between Cu(II) and DBT was −2.71 eV, higher than Ni(II) and Zn(II), and that between Cu(II) and toluene was −1.75 eV, lower than Ni(II) and Zn(II), indicating that the highest binding energy difference was responsible for the best adsorption capability. Apart from these, wave function analysis show the electron configuration between Cu(II) and DBT had the highest binding energy difference. Finally, the impact of electron configuration on adsorption performance is further investigated by modulating the electron configuration of Ni(II) to enhance/suppress its adsorption capability. According to the findings of this study, tuning the electron configuration is an effective strategy to develop materials in adsorptive desulfurization particularly for extra low sulfur content.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2016
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IF 1.207
Jianwei Li,Xiang Li,Yan Liu,Jie Zhang
The application of ionic liquids as alternatives to conventional organic solvents in the extraction process has been investigated. In the present study, fourteen species of imidazolium-based ionic liquids were added into the NaOH (aq) to remove the mercaptans. The influences of anion species and cation alkyl chain length of the imidazolium-based ionic liquids on the performance of mercaptan removal from light oils have been discussed. The efficiency of extraction for mercaptans exhibited the order of [Ac] − > [OH] − ≈ [Br] − > [BF 4 ] − . The longer alkyl chain imidazolium-based ionic liquids contributed to enhance desulfurization rate of 1-butyl mercaptan. 100% desulfurization rate of 1-butyl mercaptan was achieved by the anion of Ac − ionic liquids and NaOH (aq) at a volume ratio of 40:1 ( V (oil): V (ionic liquid)) and a short equilibrium time within 10 min.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2013
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IF 2.206
Chenhua Shu,Tonghua Sun,Jinping Jia,Ziyang Lou
A novel integrated process was proposed for reductive desulfurization of diesel fuel, in which the reductant sodium borohydride (NaBH4) was in situ generated via sodium metaborate (NaBO2) electroreduction. In order to improve the conversion rate of BO2– into BH4–, NaBO2 electroreduction was fulfilled by applying pulse voltage and using a boron-doped diamond (BDD) thin film electrode. The NaBO2 electroreduction process was analyzed by cyclic voltammetry and 11boron nuclear magnetic resonance (11B NMR) and the factors that influenced desulfurization efficiency were investigated. Under the optimal conditions desulfurization efficiency reached more than 93% for model diesel fuel. The components of model diesel fuel after desulfurization were analyzed by gas chromatography/mass spectrometry (GC/MS) and the electrolyte and digestion solution of precipitate were analyzed by inductively coupled plasma (ICP). Results indicated that B recycle was realized at the same time as desulfurization. Finally, the desulfurization of real diesel fuel was investigated. This work showed that the integrated process may be a new option for desulfurization of diesel fuel due to its mild conditions.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Frontiers of Chemical Science and Engineering
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2019
·Vol. 14
·期 4
·546-560
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IF 2.809
Wang Hanlu,Jibrin Idris,Zeng Xingye
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.
研究领域:
化学工程
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催化材料
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2021
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IF 4.311
Jingjing Li,Yijia Liang,Xiaodong Tang,Xiaojie Lei
Methane sulfonic acid (MSA) was used as anion to synthesize a series of ionic liquids and its desulfurization performance was evaluated by extraction. The basic physical properties and structural properties of the ionic liquids were evaluated, and it was proved that the ionic liquids could be used and separated well in liquid–liquid extraction desulfurization (EDS) system. The liquid–liquid extraction desulfurization system was enhanced by microchannel technology. The effects of microchannel diameter, extraction temperature, residence time and extraction stage on extraction efficiency were discussed. In the microchannel extraction system, this extraction equilibrium time can be reduced to 60 s from more than 10–15 min or longer in the conventional intermittent extraction techniques, which effectively reduces the synthesis and production cost. This finding may provide some reference for the further study of the micro-reaction technology in the deep removal of sulfur compounds from gasoline by ionic liquid, and further optimize the operating conditions.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
Chemical Engineering and Processing-Process Intensification
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2017
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IF 2.234
Shengnan Yu,Zhongyi Jiang,Weidong Li,Josue Quispe Mayta,He Ding,Yimeng Song,Zhe Li,Zhiwei Dong,Fusheng Pan,Baoyi Wang,Peng Zhang,Xingzhong Cao
Metal organic framework CuBTC nanoparticles were incorporated into polyether-block-amide (Pebax) to promote the transport of penetrant molecules in the membranes. The CuBTC nanoparticles can form hydrogen-bonds with the Pebax chains, thus interfered with the chain packing and tailored the free volume properties of Pebax. The channels and active metal sites of CuBTC promoted the transport of sulfur-containing molecules when the membranes were employed for gasoline desulfurization. When the filler content was 2 wt%, the optimal separation performance was achieved with a permeation flux of 4.4 kg/(m 2 h) and a thiophene enrichment factor of 6.0 at 40 °C, increased by 36% and 11% compared with the Pebax pristine membrane. The comprehensive performance of the membranes is more competitive than widely-used PDMS membranes, especially under high temperatures. A permeation flux of 16.45 kg/(m 2 h) is reached with an enrichment factor of 4.04 at 70 °C.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Yanchen Wei,Ming Zhang,Peiwen Wu,Jing Luo,Duanjian Tao,Chong Peng,Li Dai,Leigang Wang,Huaming Li,Wenshuai Zhu
Depending on the synthetic method, the heteroatom-doped hexagonal boron nitride (h-BN) catalysts can have different configurational entropies possessing various atomic short-range orderings or phase separations, leading to complex grain boundaries for catalytic reactions. Herein, several carbon and oxygen co-doped h-BN (BCNO) catalysts with different atomic orderings were synthesized from the ternary deep eutectic solvents (DES). The experimental results indicated the low steric resistance DES induced high-entropy structures (HES) in the BCNO, which involved a high density of grain boundaries. The HES was investigated as a catalytic booster for the radical initiation of aerobic oxidative desulfurization (ODS) of diesel. As a result, the optimized BCNO catalyzed ODS process owned the shortest induction period, rendering the complete aerobic oxidation of refractory sulfur compounds in 6 h.
研究领域:
材料科学
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催化化学
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能源化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yan Gao,Miao Yan,Liangting Chen,Jianshe Zhao
High activity peroxophosphotungstates with different organic cations were encapsulated into the metal-organic framework modified by magnetic nanoparticle (Fe 2 O 3 /MIL-101) to prepare the magnetic supported catalysts, which were used to improve the diesel desulfurization efficiency. The desulfurization result shows that one selected catalyst, (BTA) 3 PW 4 @Fe 2 O 3 /MIL-101, possesses high catalytic activity in the oxidation of various organic sulfides with H 2 O 2 as green oxidant. The catalyst can be magnetically recycled and reused for ten consecutive cycles without significant decrease in activity. Based on the GC-MS and EPR results, it is confirmed that sulfides are oxidized to corresponding sulfones in the presence of •OH radical. In a word, the high activity, good stability and reusability of catalyst prepared in this work make it have a good prospect of industrial application.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
DOI
高影响因子
Applied Sciences-Basel
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2021
·Vol. 11
·期 5
·2018
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IF 2.679
Yang Chen,Qi Tian,Yongsheng Tian,Jiawei Cui,Guanghui Wang
A mesoporous silica-supported molybdenum oxide catalyst with a cerium(Ce) modifier was prepared by in situ synthesis and used in a hydrogen peroxide (H2O2) system for the desulfurization of dibenzothiophene (DBT), benzothiophene (BT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT) fuel oils. The catalytic performance of the catalyst was studied. The catalyst was characterized by Fourier Transform Infra-Red (FT-IR), X-ray diffraction (XRD), Brunner−Emmet−Teller (BET), and X-ray Photoelectron Spectroscopy (XPS). The influences ofm(catalyst)/m(fuel oil),v(H2O2)/v(fuel oil), reaction temperature, and reaction time were investigated. The catalyst had excellent catalytic oxidation desulfurization performance under moderate operational conditions. The catalytic performance was in the order DBT > 4,6-DMDBT > BT. The kinetic analysis results showed that the reaction was a pseudo first-order kinetics process and the apparent activation energies of DBT, BT, and 4,6-DMDBT were 46.67 kJ/mol, 56.23 kJ/mol, and 55.54 kJ/mol, respectively. The reaction products of DBT, BT, and 4,6-DMDBT were DBTO2, BTO2, and 4,6-DMDBTO2, respectively. The recycling experiments indicated that DBT, BT, and 4,6-DMDBT removal could still reach levels of 94.0%, 63.0%, and 77.9% after five cycles.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
MOLECULES
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2017
·Vol. 22
·期 2
·305
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IF 2.861
Jingwei Rui,Fei Liu,Rijie Wang,Yanfei Lu,Xiaoxia Yang
A series of Zn-modified NaY zeolites were prepared by the liquid-phase ion-exchange method with different Zn sources, including Zn(NO3)2, Zn(Ac)2and ZnSO4. The samples were tested as adsorbents for removing an organic sulfur compound from a model gasoline fuel containing 1000 ppmw sulfur. Zn(Ac)2-Y exhibited the best performance for the desulfurization of gasoline at ambient conditions. Combined with the adsorbents’ characterization results, the higher adsorption capacity of Zn(Ac)2-Y is associated with a higher ion-exchange degree. Further, the results demonstrated that the addition of 5 wt % toluene or 1-hexene to the diluted thiophene (TP) solution in cyclohexane caused a large decrease in the removal of TP from the model gasoline fuel. This provides evidence about the competition through the π-complexation between TP and toluene for adsorption on the active sites. The acid-catalyzed alkylation by 1-hexene of TP and the generated complex mixture of bulky alkylthiophenes would adsorb on the surface active sites of the adsorbent and block the pores. The regenerated Zn(Ac)2-Y adsorbent afforded 84.42% and 66.10% of the initial adsorption capacity after the first two regeneration cycles.Keywords:Zeolite;Zinc sources;adsorption;desulfurization;ion exchange
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
PubMed
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
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2016
·
IF 1.083
Chenhua Shu,Tonghua Sun
In this study, three tetrabutyl ammonium chloride (TBAC)-based deep eutectic solvents (DESs) were synthesised and used for desulfurising model and real gasolines. Extraction efficiencies of different DESs followed the order of TBAC/ethylene glycol > TBAC/glycerol > TBAC/malonic acid. After five extraction cycles, the extraction efficiencies of TBAC/ethylene glycol, TBAC/glycerol and TBAC/malonic acid reached 99.5, 99.3 and 99.2%, respectively. Additionally, the structures of original and recycled DESs were analysed and the results showed that DESs maintained their original structures after regeneration. Finally, the desulfurisation performance of DESs for real gasoline was also investigated. This work will provide new green extractants for gasoline desulfurisation.
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
ENERGY & FUELS
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2015
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IF 2.79
Xiao-dong Tang,Tao Hu,Jing-jing Li,Fang Wang,Da-yong Qing
To meet the environmental requirements, kerosene, as the major component of jet fuel, is necessary for deep desulfurization. An electrochemical oxidation–extraction method was proposed to reduce the sulfur content in kerosene in this work. First, the electrochemical oxidation of kerosene was carried out in NaCl solution. Then, N-methyl-2-pyrrolidone (NMP) was used as an extractant to remove the oxidized organic sulfides. Gas chromatography–flame photometric detector (GC–FPD), gas chromatography–mass spectrometry (GC–MS), Fourier transform infrared (FTIR) spectroscopy, and ion chromatography were used to determine 1-heptyl mercaptan, one of the main organic sulfides in kerosene, and its products after electrochemical oxidation. The results showed that 1-heptyl mercaptan was effectively oxidized to diheptyl disulfide, 1-heptanesulfonyl chloride, and sulfate in electrochemical oxidation and removed after extraction. After electrochemical oxidation–extraction, the sulfur content of kerosene decreased from 180.0 to 13.2 μg/g and the desulfurization efficiency reached 92.67%. By gas chromatography–flame ionization detector (GC–FID) analysis of kerosene, the electrochemical oxidation process has no impact on the properties of kerosene. On the basis of these experimental results, a mechanism of electrochemical oxidative desulfurization was proposed.
研究领域:
环境科学
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能源化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）