FUEL
·
2016
·
IF 3.611
Wei Jiang,Dan Zheng,Suhang Xun,Yuejiao Qin,Qingqing Lu,Wenshuai Zhu,Huaming Li
A supported heterogeneous catalyst with polyoxometalate-based ionic liquid (POM-IL) [N-(3-sulfonatepropyl)-pyridinium] 3 PMo 12 O 40 ([PSPy]PMo) served as active component was prepared and graphite carbon (GC) with layer structure was used as support. Characterizations of the supported catalyst by FT-IR, Raman, XRD, XPS and TEM confirmed that IL was immobilized on GC successfully and the structure was retained after the hydrothermal impregnation method. The as-prepared catalyst exhibited high catalytic performance in the solvent-free oxidative desulfurization system. Various of reaction conditions were investigated and the removal of dibenzothiophene reached 100% under the optimum conditions. Wettability experiments and kinetics studies were taken to better understand the oxidation reactions. In addition, the suggested mechanism was given with the help of Gas Chromatography–Mass Spectrometer analysis. Moreover, the supported catalyst had a good recyclability, which made it have a promising prospect for industrial application.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Fa-tang Li,Biao Wu,Rui-hong Liu,Xiao-jing Wang,Lan-ju Chen,Di-shun Zhao
Inexpensive N-methyl-pyrrolidone (NMP)-based ionic liquids (ILs) are synthesized by coordinating N-methyl-pyrrolidone with anhydrous FeCl 3 or ZnCl 2 . The introduction of metal chlorides lowers the solubility of NMP for actual diesel. The obtained C 5 H 9 NO·0.3FeCl 3 IL shows remarkable extraction ability for dibenzothiophene (DBT) with Nernst partition coefficients ( k N ) above 7.5, which can be attributed to its low viscosity and bifunctional extractive groups of five-membered ring of NMP and unoccupied orbitals of Fe ion. The oxidative desulfurization of DBT using H 2 O 2 as oxidant and ILs as extractants are investigated. The scavenger experiments and electron paramagnetic resonance (EPR) measurement verify the active species is hydroxyl radical ( OH) responsible for the oxidation of DBT. FeCl 3 -based ILs show much better effects in catalyzing H 2 O 2 to generate OH than ZnCl 2 -based ILs. The process and mechanism for extraction and catalytic oxidation of DBT in an oil–ionic liquid–H 2 O 2 system are proposed. The C 5 H 9 NO·0.3FeCl 3 IL shows excellent recycling performance. After six-run experiment, there is only little loss in activity, which can be ascribed to the high solubility (18,190 ppm) of dibenzothiophene-sulfone (DBTO 2 ), the main oxidation product of DBT, in the IL.
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ChemSusChem
·
2017
·Vol. 10
·期 8
·1669-1674
·
IF 7.226
Zhongsen Ma,Hualei Hu,Zhongqiang Sun,Wenting Fang,Jian Zhang,Longfei Yang,Yajie Zhang,Lei Wang
Graphical Zeolite catalysis : Zeolite L is synthesized by the hydrothermal method, post-treated by NH 4 exchange to adjust its acidity, and characterized by various techniques. In the dehydration of fructose catalyzed by modified zeolite L in the ionic liquid [bmim]Br, 99.1 % yield of 5-hydroxymethylfurfural (HMF) is obtained. Zeolite L was synthesized by the hydrothermal method and post-treated by NH 4 exchange to adjust its acidity. The samples were systematic characterized by various techniques including XRD, X-ray fluorescence spectroscopy, N 2 adsorption–desorption, scanning electron microscopy, pyridine IR spectroscopy, and NH 3 temperature-programmed desorption. The results demonstrated that the NH 4 -exchange post-treatment increased the surface area, micropore volume, and acidity of zeolite L. The catalytic performance of the samples was tested in the dehydration of fructose to 5-hydroxymethylfurfural (HMF) in ionic liquid (1-butyl-3-methylimidazolium bromide, [bmim]Br). 99.1 % yield of HMF was obtained when the KL-80 °C-1 h sample (KL zeolite treated with 1 m NH 4 NO 3 solution at 80 °C for 1 h) was used. The high efficiency could be attributed to the appropriate acid properties of the catalyst. The zeolite catalyst could be reused four times without significant decrease in activity.
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ChemCatChem
·
2024
·
IF 3.8
Hongyu Zhang,Shaojuan Zeng,Chongyang Jiang,Kuilin Peng,Jiaqi Feng,Lei Yuan,Xin Li,Fei Xu,Xiangping Zhang
The application of electrochemical CO2 reduction reaction (CO2RR) to generate value-added products, including carbon monoxide (CO), represents a sustainable strategy for addressing the global carbon balance. Silver (Ag) has gained significant attention as an attractive and cost-effective electrocatalyst for CO2RR-to-CO due to high activity. Here, the porous Ag nanofoam catalysts with Ag(111)-dominant were prepared by in-situ electrolysis-deposition method in the ionic liquid (IL) electrolyte. The Ag nanofoam catalysts exhibited exceptional activity in converting CO2 to CO, with a high Faradaic efficiency (> 95%) in a wide range of -1.9 ~ -2.4 V vs. Ag/Ag+ in the 1-butyl-3-methylimidazolium tetrafluoroborate ([Bmim][BF4]) electrolyte. The maximum CO partial current density of -125.40 mA cm-2 was obtained on this Ag nanofoam catalyst, representing 62% improvement over Ag(110)-dominant Ag electrode (-77.35 mA cm-2) at -2.4 V vs Ag/Ag+ in the [Bmim][BF4] electrolyte. Density functional theory calculations demonstrate that the Ag(111) crystal facet formed by in-situ electrolysis-deposition method prefers to adsorb [Bmim][BF4] which can stabilize the reaction intermediate, thereby weakening the reaction free energy and promoting CO2 electroreduction.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Liu,Chao Pan,Xianjie Li,Hailin Zhang,Zhijie Shang,Hongbing Song
Oxidation, a pivotal process in organic synthesis, is essential for the conversion of various biomass derivatives, including 5-hydroxymethylfurfural (HMF), into valuable chemicals. This research employs poly(ionic liquid)s (PILs) as supports to fabricate Au/PILs catalysts, which are subsequently utilized in the oxidative esterification of HMF to produce dimethyl 2,5-furandicarboxylate (FDMC). The modification of PILs demonstrates that catalyst’s performance is optimized when the PILs anion (IL: EGDMA = 1: 4) is [Tf 2 N - ]. The presence of the [Tf 2 N - ] group is essential for charge transfer between the carrier and the active metal Au, thereby enhancing the catalytic reaction. Thermogravimetric analysis (TG) reveals the exceptional thermal stability of the 2 % Au/PILs-Tf 2 N-14 catalyst. The efficient conversion of HMF to FDMC is achieved using the 2 % Au/PILs-Tf 2 N-14 catalyst at 120°C, 12 h, with CH 3 ONa (0.75 equiv.) and 2 MPa O 2 , yielding a HMF conversion ( C HMF ) of 96.41 % and a FDMC selectivity ( S FDMC ) of 100 %. The heterogeneous catalyst 2 % Au/PILs-Tf 2 N-14 maintains high catalytic activity after multiple cycling experiments. A catalyst based on precious metal-loaded PILs was utilized to achieve efficient and selective conversion of HMF to FDMC under low loading conditions. This approach not only offers valuable insights for future research but also promotes the shift towards renewable energy sources. Additionally, the adsorption behavior of O 2 on Au 8 clusters and the interaction between the reaction substrate HMF and [Tf 2 N - ] were examined through density functional theory (DFT) calculations, providing theoretical backing for further investigation.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Zhanjun Li,Yunwei Liu,Mingru Kong,Yibin Xu,Kunlun Wang,Ke Ma,Qi Shen,Qingfen Zhang
To increase the extraction efficiency of quercetin from Pinus koraiensis seed scales (PKSS), an innovative chitosan-Cu-Fe (CS-Cu-Fe) ionic liquid system for efficient ultrasonic-assisted extraction (UAE) of PKSS quercetin (PKSSQ) was designed. A first-order kinetic model was applied to analyse the extraction performance, and key factors influencing the process were systematically optimized. The optimal conditions were as follows: 2.00 g sample, 0.016 mol [BMIM]Br, 0.6 %, 100 W, 53°C, 12:1 mL/g, and 14 min. Under these conditions, the actual PKSSQ yield was 2.92 mg/g ± 0.02 mg/g, which closely aligned with the theoretical yield of 2.96 mg/g. The extraction kinetics were compared across different methods, and the stability of the CS-Cu-Fe system was evaluated through recovery experiments. The CS-Cu-Fe was characterized using Fourier transforms infrared (FT-IR) spectroscopy, thermogravimetric analysis (TGA), X-ray diffraction (XRD), hysteresis loop (HL) measurement, electrical conductance (EC) measurement and scanning electron microscopy (SEM) of the extracted residues. CS-Cu-Fe demonstrated exceptional thermal stability, magnetic properties, and catalytic activity, significantly enhancing the PKSSQ extraction efficiency. FT-IR analysis revealed minimal spectral changes in CS-Cu-Fe, with notable EC differences. Owing to its stable core functional groups, CS-Cu-Fe maintained excellent thermal stability, crystal structure, soft magnetism, and catalytic efficiency. This study highlights the efficiency of the CS-Cu-Fe ionic liquid system in UAE of PKSSQ and the role of its stable core functional groups in improving the extraction and catalytic performance. This innovative approach provides a robust theoretical foundation for extracting and developing natural products from PKSS, with promising future applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jun Li,Jianwei Zhang,Yingzhe Du,Xiaoxia Liu,Ronghao Liu,Yanzhao Yang
Efficient gold extraction is of paramount importance, but how to improve the extraction efficiency and enhance the driving force of the extraction process is still to be explored. This study introduces an innovative approach using versatility ionic liquids (ILs) to overcome existing challenges. A tailored IL was synthesized and employed computational tools, including the Interaction Region Indicator, to predict its effectiveness in gold extraction. Quantum chemical calculations elucidated the interplay between hydrogen bonding capability and ion exchange properties of the ILs. Subsequent optimization of experimental conditions (0.1 mol/L HCl, 10.6 mg IL) yielded a remarkable 98.4 % extraction efficiency at 45 °C. Molecular dynamics simulations affirmed the IL's exceptional selectivity for Au(III) extraction, with analysis revealing that the extraction mechanism primarily hinged on electrostatic attraction and van der Waals interactions between ionic liquid cations and [AuCl 4 ] − . This mechanism aligns with the established anion exchange mechanism, validated through Ultraviolet–visible spectrometer (UV–Vis), Nuclear Magnetic Resonance spectrometer (NMR), and Liquid Chromatograph Mass Spectrometer (LC-MS) analyzes. To complete the extraction cycle, 1.0 mol/L K 2 C 2 O 4 was employed as a stripping agent for efficient Au(III) recovery from the loaded IL phase, facilitating repeated extraction cycles. This study underscores the sustainability of the IL-based Au(III) extraction process, maintaining consistently high extraction rates even after five cycles. In summary, this method does not use solvent, enabling environmentally friendly Au(III) extraction.
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Catalysts
·
2025
·Vol. 15
·期 3
·279
·
IF 4
Duozhen Chai,Chongli Wang,Jinzhen Liu,Dongfeng Cao,Kaixuan Guo,Yuankun Wang,Ye Yuan,Francis Verpoort
The cyclization of propargyl alcohols with CO2represents a highly significant method for the utilization of CO2. The resulting cyclic carbonates possesses high chemical value and hold great potential for applications in battery electrolytes, polymer precursors, and pharmaceutical intermediates. However, most existing reports on this cyclization have been limited to simple propargyl alcohol substrates that are substituted with inert alkyl, cycloalkyl, and phenyl groups. For functionalized propargyl alcohols, such as alkyne-1,2-diols, only a single report has been documented thus far. In this study, we have developed an innovative catalytic system comprising cost-effective copper salts and environmentally friendly ionic liquids (CuCl/1-ethyl-3-methylimidazolium acetate) for the cyclization of alkyne-1,2-diols with CO2. Compared to the previously reported AgF/bulky monophosphine ligand (BrettPhos) system, our system is free of traditional volatile solvents, phosphine ligands, and additives. Notably, this is the first reported Cu(I)-catalyzed system for this cyclization, offering significant advantages in terms of cost-effectiveness and reduced toxicity compared to silver salts. Moreover, the use of ionic liquids ensures considerable recyclability, further enhancing the sustainability and practicality of this approach.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Li-Hao Xu,Yan Li,Shen-Hui Li,Heng Mao,Zhi-Ping Zhao
The application of membrane-based separation technology in purifying azeotropic solutions plays a crucial role in minimizing energy consumption during reactive distillation. The strategic integration of multi-dimensional structural composites within mixed matrix membranes (MMMs), characterized by a robust framework and efficient molecular transport channels, poses challenges but demonstrates significant potential for advancing the development of high-performance membrane fabrication. Herein, we proposed a novel strategy to covalently assemble halloysite nanotubes (HNTs) and graphene oxide (GO) using ionic liquids (ILs) as linkers. When incorporated into the polyvinyl alcohol (PVA) matrix, the ILs@HNTs@GO (IHGO) composites exhibit excellent interfacial compatibility, and ILs also enhanced the composite’s selective transfer ability to water molecules. The optimal separation performance for pervaporation dehydration from a ternary solution was respectively 2.57 (selectivity) and 1.74 (permeability) times higher than those of the pristine PVA membrane. The structural stability of the MMMs and their separation mechanism has been comprehensively validated by adjusting the content of GO in IHGO composites and conducting simulations. This study holds significant theoretical and practical implications for organic compounds purification, while simultaneously paving new avenues for the fabrication of structurally robust and high-performance MMMs with optimal filler effectiveness.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lingwang Liu,Jiangyan Xue,Yang Liu,Suwan Lu,Shixiao Weng,Zhicheng Wang,Fengrui Zhang,Daosong Fu,Jingjing Xu,Xiaodong Wu
Polymerized ionic liquid (PIL)-based gel polymer electrolytes (GPEs) are well known as highly safe and stable electrolytes but with low ambient ionic conductivity. Herein, we first designed and synthesized an IL monomer with a long and flexible side chain and then mixed it with LiTFSI and MEMPTFSI to construct a PIL-based GPE (denoted as GM-GPE). The special molecular structure of the monomer greatly improves the ionic transport through the PIL chain, and the introduction of MEMPTFSI plasticizer further improves the ionic conductivity, promoting a TFSI–-anion-derived SEI formation to suppress Li dendrite growth and forming an electrostatic shielding effect of MEMP+ cations to promote the uniform deposition of Li+. Consequently, the as-prepared GM-GPE exhibits high ambient ionic conductivity (4.3 × 10–4 S cm–1, 30 °C), robust electrochemical stability, excellent thermal stability, nonflammability, and superior ability to inhibit Li dendrite growth. The resultant LiFePO4|GM-GPE|Li cell exhibits a high discharge capacity of 150 mA h g–1 at 0.2 C along with a good cycling stability and rate capability. This work brings about new guidance for the development of high-quality GPEs with high ionic conductivity, high stability, and safety for long cycling and dendrite-free lithium metal batteries.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 26
·11776-11782
·
IF 2.7
Yuwei Yan,Hongyan Li,Songnan Li,Jiawei Zhang,Jingxiang Zhao,Qinghai Cai
Copper, iron–chloride ionic liquids (ILs) were immobilized on SBA-15 via N-methylimidazole grafting with C–Cl in chloropropylsilane pre-anchored on SBA-15, followed by FeCl3 and CuCl2 coordination to imidazolium chloride to generate a double metal IL-supported mesoporous composite (SIL-CuFe). The prepared composite exhibited an effective catalytic performance for the solvent-free oxidation of styrene to benzaldehdye (BzH) with H2O2 oxidant, offering 51% conversion, a turnover number (TON) of 330.5 mol molFe+Cu−1, and a selectivity of 71% at a reaction temperature of 70 °C. The composite catalyst can be easily recovered and effectively reused without a significant loss in activity and selectivity. The quenching experiments by adding tert-butanol (TBA), 1,4-benzoquinone (p-BQ) and L-histidine (L-HIS) in the reaction system were conducted to identify the type of reactive O species, specifically ˙OH, ˙O2−, and 1O2, produced by catalyst activation with H2O2 and played a main role in the oxidation. The reaction mechanism of the oxidation process is also proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hong Chen,Jindong Huang,Chao Zhang,Peng Gao,Hongchang Huang,Junlan Li,Juncheng Liu
A foldable polyimide (PI) protective layer with high transmittance and high ultraviolet (UV) resistance is crucial for the practical application of flexible solar cells. Herein, the commercially 2,2′-Bis(trifluoromethyl) benzidine (TFMB) and 4,4′-(hexafluoroisopropylidene) diphthalic anhydride (6FDA) as the monomers, and five ionic liquids (ILs) as the regulators were used to synthesize PI/IL films (PI/IL1, PI/IL2, PI/IL3, and PI/IL4). The outcomes reveal that the average transmittance ( AT ) of PI/IL1 (50 μm thickness) outperforms others, which can be attributed to the expanded π-π stacking distance between PI molecules and the intermolecular multipoint interaction between IL1 and PI. The AT and the elongation at break ( ε ) of PI/IL1 increase sequentially with the 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C 2 mim][NTf 2 ])/TFMB mole ratio, and those of PI/IL1-3 reach the maximum values of 94.23 % and 49.42 % at a 3:1 ratio, respectively. However, the tensile strength ( σ ) of the PI/IL1 film is inferior to that of the pure PI film, and consistently decreases with the increase of [C 2 mim][NTf 2 ]/TFMB mole ratio. Nevertheless, the UV-induced degradation of PI can be delayed through the [C 2 mim][NTf 2 ] regulation. The attenuations of AT , σ and ε of PI/IL1-3 films after 1000 equivalent solar hours (ESHs) UV irradiation are 0.85 %, 14.63 % and 2.99 %, respectively, which are significantly lower than those of pure PI films (2.23 %, 32 % and 23 %). This is attributed to the interaction between the positive and negative charges from [C 2 mim][NTf 2 ] and those from the PI chain breaking. The highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of PI/IL1-3 are calculated with the density functional theory to reveal the charge transfer between [C 2 mim][NTf 2 ] and PI.
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