FUEL
·
2018
·
IF 4.908
Hang Xu,Dandan Zhang,Fengmin Wu,Xuefeng Wei,Jun Zhang
Deep eutectic solvents (DESs) are receiving increasing attention as ionic liquid analogues because of their environmentally friendly and very low-price characteristics. In this study, metal-based deep eutectic solvents (MDESs) were synthesized by combining cobalt chloride (CoCl 2 ), a hydrogen bond acceptor (HBA) such as choline chloride (ChCl), and hydrogen bond donors (HBDs) such as polyethylene glycol (PEG-200), ethylene glycol (EG), glycerol (GL), and propionic acid (Pr). The MDESs were used for the extractive catalytic oxidative desulfurization (ECODS) of fuels. Solid peroxymonosulfate (PMS) was selected as an oxidant over common ECODS oxidants such as liquid hydrogen peroxide because the former is cheaper, more stable, and less corrosive. The MDESs played dual roles (i.e., extractant and catalyst) during the ECODS process. One of the MDESs prepared (CoCl 2 -ChCl/2PEG) showed fast reaction rates with nearly 100% dibenzothiophene removal under the optimal conditions (6 g of model oil with an initial sulfur content of 500 ppm, 0.9 g of PMS solution, 2 g of CoCl 2 -ChCl/2PEG, 20 °C, and 60 min). The DESs prepared showed an outstanding recycling performance after 6 cycles without a significant decrease in activity. In the ECODS system, the reactivity of the three sulfur substrates studied followed the order: dibenzothiophene (DBT) > 4,6-dimethyldibenzothiphene (4,6-DMDBT) > benzothiophene (BT). In the case of the HBDs, the desulfurization efficiencies followed the sequence: PEG-200 > Pr > EG > GL. The oxidative product was dibenzothiophene sulfone (DBTO 2 ).
研究领域:
化学工程
·
环境科学
·
催化材料
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Xiao-Xiao Xing,Hui-Li Guo,Tong Feng,Tian-Meng He,Wen-Shuai Zhu,Hua-Ming Li,Jing-Yu Pang,Yan Bai,Dong-Bin Dang
Achieving long-term stable deep desulfurization at room temperature and recovering high value-added sulfone products is a challenge at present. Herein, a series of catalysts [Cnmim]5VW12O40Br (CnVW12, 1-alkyl-3-methylimidazolium bromide tungstovanadate, n = 4, 8, 16) were presented for the room temperature catalytic oxidation of dibenzothiophene (DBT) and its derivatives. Factors affecting the reaction process, such as the amount of catalyst, oxidant, and temperature, were systematically discussed. C16VW12 showed higher catalytic performance, and 100% conversion and selectivity could be achieved in 50 min with only 10 mg. The mechanism study showed that the hydroxyl radical was the active radical in the reaction. Benefiting from the “polarity strategy”, the sulfone product accumulated after 23 cycles in a C16VW12 system, and the yield and purity were about 84% and 100%, respectively.
研究领域:
化学
·
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 8
·3605-3626
·
IF 3.3
Li Xing,Huhe Taoli,Zeng Tao,Ling Xiang,Huang Hongyu,Chen Yong
Carbon materials mainly capture sulfur dioxide (SO 2 ) from gas through physical adsorption, therefore their SO 2 capture performance will decrease with the increase in desulfurization temperature. In order to meet the stringent requirements of deep desulfurization, further improvements on carbon materials are necessary, improving their SO 2 capture performance and adaptability to changes in desulfurization temperature. In this study, a carbon material (NCP10) was modified with various alkali metal compounds with the aim of enhancing the SO 2 capture performance and adaptability to temperature changes. The results showed that the NCP10/LiOH composite had the best average SO 2 removal rate (100%) and SO 2 capture capacity ( \({113}.{6} \;{\text{mg}}_{{{\text{SO}}_{2} }} /{\text{g}}_{{{\text{material}}}}\) ) within the first hour of reacting at 60 °C, the SO 2 removal rate and SO 2 capture capacity of the NCP10/LiOH composite were 29% and 29% higher than those of the pure NCP10 material, respectively. While the SO 2 capture performance of the NCP10 modified with LiCl, Li 2 CO 3 , NaOH and KOH were not sufficient for deep desulfurization, the SO 2 capture performance of the NCP10/LiOH(2:1) composite was able to meet the requirements of deep desulfurization in the temperature range of 25–100 °C by the physical adsorption and chemical absorption synergistically effect.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2017
·Vol. 34
·期 12
·3132-3141
·
IF 2.007
Zhang Wei,Li Xin,Wang Hong,Song Yongji,Zhang Shenghong,Li Cuiqing
Deep desulfurization of model oil by photocatalytic air oxidation and adsorption using Ti (1− x ) M
x
O 2 (M=Zr, Ce) was investigated. Ti (1− x ) M
x
O 2 (M=Zr, Ce) was prepared by urea gelation/co-precipitation method, and characterized by N 2 adsorption, XRD and UV-vis spectra. UV irradiation greatly enhanced the adsorptive capacity and selectivity of TiO 2 -ZrO 2 for organosulfur in model oil because organosulfur compounds were first photocatalytically oxidized to sulfoxides and sulfones over TiO 2 -ZrO 2 , which were then selectively adsorbed on the bifunctional material due to much higher polarities of generated sulfoxides and sulfones. The Ti/Zr molar ratio and calcination temperature were optimized to 5 : 5 and 500 °C with the sulfur removal of 99.6% after reaction for 2 h under UV irradiation. After adding 25 wt% toluene into model oil, the sulfur removal could still reach 97.2% after reaction for 7 h. TiO 2 -ZrO 2 could be well regenrated by washing with acetonitrile followed by thermal treatment in air.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2015
·
IF 2.337
Zhen Song,Teng Zhou,Jianan Zhang,Hongye Cheng,Lifang Chen,Zhiwen Qi
When applying ionic liquids (ILs) for solvent-sensitive extraction systems, ILs dissolved in the raffinate may lead to severe subsequent problems or a significant reduction in product quality, and thus should be particularly concerned. To screen qualified IL solvent for such systems, a rigorous criterion considering both its solubility in the raffinate and extractive ability is established. The COSMO-RS model is used to evaluate the effect of anions and cations, and suggest potential ILs meeting the criterion. Afterwards, the solubility and extractive ability of candidate ILs are investigated by experiments to further confirm their suitability. The proposed solvent screening method is exemplified for the extractive desulfurization process. [C 4 mim][H 2 PO 4 ] is pre-selected by the screening method, and its high extractive performance is experimentally verified.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Jing He,Shuaishuai Zhou,Peiwen Wu,Yingcheng Wu,Lianwen He,Linhua Zhu,Wenshuai Zhu,Huaming Li
The interface properties of metal oxides considerably affect the catalyst activity during the removal process of persistent organic sulfur pollutant in diesel fuels. Herein, we report that the hydrophilicity of defective metal oxides can be well shielded by refining the interface. As a proof of point, multi-walled carbon nanotubes (CNTs) were employed as a solid modifier to be wound on the Mo-doped W 18 O 49 nanowire clusters (MoWO- x @CNTs) for enhanced catalytic performance. The results show that the full conversion of dibenzothiophene is achieved within 12.5 min. The turnover frequency value is up to 79.7 h −1 , much higher than other catalysts. Compared with the bare W 18 O 49 , the MoWO- x @CNTs exploits a rough hierarchical structure, which overcomes the limitation of the hydrophilic W 18 O 49 interface. Furthermore, the persistent organic sulfur in diesel fuels is <6.2 ppm, achieving the goal of ultra-deep desulfurization . Besides, no more secondary extraction is required, which also alleviating environmental pollution caused by the abuse of organic waste.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Green Energy & Environment
·
2024
·
IF 10.7
Ping Lu,Zhenhua Sun,Xinrong Ke,Changshen Ye,Zhixian Huang,Ting Qiu
Designing efficient adsorbents for the deep removal of refractory dibenzothiophene (DBT) from fuel oil is vital for addressing environmental issues such as acid rain. Herein, zinc gluconate and urea-derived porous carbons SF-ZnNC- T ( T represents the carbonization temperature) were synthesized without solvents. Through a temperature-controlled process of “melting the zinc gluconate and urea mixture, forming H-bonded polymers, and carbonizing the polymers,” the optimal carbon, SF-ZnNC-900, was obtained with a large surface area (2280 m 2 /g), highly dispersed Zn sites, and hierarchical pore structures. Consequently, SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of 43.2 mg S/g, compared to just 4.3 mg S/g for the precursor. It also demonstrated good reusability, a fast adsorption rate, and the ability for ultra-deep desulfurization. The superior DBT adsorption performance resulted from the evaporation of residual zinc species, which generated abundant mesopores that facilitated DBT transformation, as well as the formation of Zn-N x sites that strengthened the host-guest interaction (Δ E = -1.466 eV). The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Xiao Teng,Bo Zhang,Luxia Yin,Wanyi Tao,Zhang Wen,Zekai Zhang,Wensheng Ning
A series of PdO/CeO 2 /SiO 2 -z aerogel composites with different molar ratio of Si/Ce were facilely fabricated via sol-gel method combined with atmospheric drying technology, where a major of Ce 3+ species could be oxidized to Ce 4+ species by adding hydrogen peroxide. They were used to remove thiophenics from model fuels and aromatics, compared with PdO/SiO 2 and CeO 2 /SiO 2 aerogel composites. Adding Ce and Pd led to an appearance of weak Lewis acid centers on the surface of adsorbents. Compared with PdO/SiO 2 and CeO 2 /SiO 2 , the adsorption capacity of PdO/CeO 2 /SiO 2 -z significantly increased, in which PdO/CeO 2 /SiO 2 -100 performed best and the adsorption capacity for thiophene was 15.0 mg-S/g ads , which was about the sum of PdO/SiO 2 -636 and CeO 2 /SiO 2 -100. The case was attributed to π-complexation of Pd 2+ and S-M (Pd, Ce, acted as Lewis acid centers) bond (σ) with thiophenics, where the adsorption process was dominated by S–Ce bond. Combined with the same chemical state of Pd and Ce in single metal and bimetal adsorbents verified by XPS , it can be deduced that no synergistic interaction between Pd and Ce species was formed in the adsorption process. PdO/CeO 2 /SiO 2 -100 exhibited a higher resistance for competitive adsorption of aromatics and a good solvent washing regeneration performance. The adsorption process of PdO/CeO 2 /SiO 2 -100 for thiophene was well fitted by Langmuir isothermal and pseudo-secound-order model and were spontaneous and endothermic. The solvents (n-heptane, benzene and p-xylene) have no obvious effect on the adsorption thermodynamics and kinetics of PdO/CeO 2 /SiO 2 -100.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 48
·42402-42412
·
IF 3.289
Suhang Xun,Dan Zheng,Sheng Yin,Yuejiao Qin,Ming Zhang,Wei Jiang,Wenshuai Zhu,Huaming Li
A series of TiO2 microspheres supported polyoxometalate-based ionic liquids (POM-ILs) with different tungsten–titanium molar ratios and different carbon chains ILs were successfully prepared. The supported catalysts were characterized by TG, FT-IR, Raman, Nitrogen adsorption–desorption isotherms, XPS and SEM. It is confirmed that the POM-ILs were indeed immobilized on TiO2 microspheres and the structures were maintained. The appropriate morphology and loading of the supported catalyst was obtained with [C16mim]4SiW12O40 (C16SiW) IL and the tungsten–titanium molar ratio was 0.1 (0.1-C16SiW–TiO2). This heterogeneous catalyst strategy makes the usage of ionic liquid decrease sharply. The supported catalyst 0.1-C16SiW–TiO2 exhibited high catalytic activity in the extractive coupled catalytic oxidative desulfurization (ECODS) system under mild conditions. The removal of dibenzothiophene (DBT) reached 95.3% with low-dosage oxidant (the molar ratio of H2O2 and DBT is only 2), which means high efficiency utilization of H2O2 was achieved in this system. Moreover, DBT could be removed completely with a little excess oxidant. Furthermore, the 0.1-C16SiW–TiO2 catalyst showed excellent reusing ability, the desulfurization efficiency had no obvious decrease after recycling for 8 times, which made it a promising catalyst in oxidative desulfurization process.
研究领域:
化学工程
·
催化材料
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Yan Gao,Xiayu Lia,Shuai Huang,Na Zhao,Jianshe Zhao
Three-dimensionally ordered macro-microporous 3DOM-ZIF-8-based peroxophosphotungstate (DIL-PW 4 ) is constructed to break the limitation of micropores inherent in traditional supported catalysts. The presence of ordered macropores expose more active sites and significantly enhance mass diffusion, thereby boosting catalytic activity, especially in reactions involving larger molecules. The prepared composite DIL-PW 4 @3DOM-ZIF-8 is verified by various characterization techniques and used as a catalyst for the extraction oxidation desulfurization of multi-component simulated fuel. The results showed that heterogeneous catalyst DIL-PW 4 @3DOM-ZIF-8 has a remarkable catalytic effect, with 97.03% total sulfides removal in 120 min. In addition, the stability and reusability of the catalyst DIL-PW 4 @3DOM-ZIF-8 are evaluated as important parameters for industrial applications. In addition, a possible mechanism based on experimental studies are proposed.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）