Journal of CO2 Utilization
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2022
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IF 8.321
Yupeng Chen,Chong Chen,Xue Li,Nengjie Feng,Lei Wang,Hui Wan,Guofeng Guan
Catalytic fixation of greenhouse gas CO 2 into value-added chemicals under mild conditions was deemed as an effective pathway for carbon emissions mitigation, though facing big challenges. Herein, a novel hydroxyl-ionic liquid functionalized metalloporphyrin (ZnTpyp-IL) catalyst bearing hydrogen bond donor (HBD), Lewis acidic and nucleophilic sites was fabricated and invested in the CO 2 cycloaddition without additive or solvent. The integration of ionic liquid endowed the framework with strong surface affinity to enrich CO 2 molecules, while the cooperative interplay of multiple active sites further promoted the high-selective conversion of epichlorohydrin (ECH). Under optimal conditions (100 °C, 1 MPa, 4 h), the yield of corresponding chloropropene carbonate (CPC) reached 97.1 % (turnover frequency (TOF) = 52.4 h -1 ), far superior to that of bare Tpyp (17.4 %). The preliminary kinetic studies revealed the lower activation energy (59.54 kJ/mol) needed to be overcome in the ring-opening process over ZnTpyp-IL. Moreover, a plausible dual-activation mechanism of hydrogen bonds and Zn centers for epoxides was proposed based on the density functional theory calculation (DFT) to explain the acceleration of rate-determining step. Coupled with the satisfactory reusability and substrate expansibility, the developed ZnTpyp-IL demonstrated its great potential as robust heterogeneous catalyst in the efficient utilization of C 1 resource.
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Nano Energy
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2022
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IF 19.069
Yuhao Hu,Yunfei Teng,Yue Sun,Pei Liu,Lin Fu,Linsen Yang,Xiang-Yu Kong,Qiang Zhao,Lei Jiang,Liping Wen
The development and utilization of salinity gradient energy are of great significance to the carbon-neutral strategic demand for clean energy in the new era. Conventional ion-exchange membranes have been employed to recover this wide-distributed energy by reverse electrodialysis membrane processes, however, the dense membrane structure and chemical instability limit the ionic transport in various working environments. Here, inspired by the rapid mass transport caused by the hierarchical structure of blood vessels, we employ two types of polyelectrolytes to fabricate a bioinspired three-dimensional interconnect porous membrane by simply casting-soaking, and this membrane shows great chemical stability due to the ionic crossing enhancement. The interconnected nanoporous structure and the enriched surface functional groups of the membrane render the high-performance osmotic energy conversion from different resources, including the Gibbs free energy between seawater and riverwater, commonly used organic solvents , and also in the solution treatment process of spent batteries . We believe this chemical-stable, nanoporous and freestanding membrane might take one more step towards practical applications and membrane technology.
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CATALYSIS LETTERS
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2022
·Vol. 153
·期 1
·271-284
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IF 2.936
Faizan Muhammad,Zhang Ruirui,Liu Ruixia
Recently, global warming is proving to be an increasing challenge for the sustainable human survival on planet earth. Worldwide, researchers are putting their efforts into controlling carbon emissions and have set the aim to achieve levels of overall carbon neutrality. Different industrial processes, especially oil refinery processes, release large amounts of low-carbon alkanes as gaseous byproducts directly into the air and pollute clean environments, which is one of the major reasons for sudden climate changes, ocean acidification, loss of biodiversity, and rising sea levels. The conversion of lighter alkanes, especially n-butane, into value-added chemicals can be beneficial for green economies and green environments. Presently, heterogeneous vanadium phosphorus oxide catalysts (VPOs) are considered potential candidates for n-butane selective oxidation toward maleic anhydride (MA). In this research, we developed a VPO catalyst with the assistance of copper-based ionic liquids (Cu-ILs), including [Bmim][OAc]–[Cu(OAc) 2 ], [Bmim][Cl]–[CuCl], and [Bmim][Cl]–[CuCl 2 ]. We observed significant improvement in the MA selectivity; meanwhile, the CO x (CO and CO 2 ) selectivity was decreased. Compared to the unpromoted catalyst (Blank-VPO), the Cu-IL-promoted catalyst, i.e., [Bmim][Cl]–[CuCl 2 ]-VPO remarkably increased the MA selectivity (11%) and n-butane conversion (9.2%) and minimized the CO x selectivity (11%). In addition to this the ratio of CO/CO 2 has been reduced from 2.01 to 1.32. Therefore, this can be a helpful process for achieving carbon neutrality goals. Graphical Abstract
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Materials
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2022
·Vol. 15
·期 7
·2628
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IF 3.748
Yafei Liu,Yiyu Shi,Yan Cui,Fen Zhao,Mindong Chen
Magnetic polymers are often used as loading materials for ionic liquids because of their excellent magnetic separation properties. In this study, a novel imidazolium-based ionic liquid-modified magnetic polymer was synthesized by suspension polymerization and grafting, denoted as γ-Fe2O3@GMA@IM, and this magnetic polymer was used for the adsorption of the acid dye FCF. The magnetic polymer was characterized by SEM, FTIR, XRD, VSM and TGA. These techniques were used to reveal the overall physical properties of magnetic polymers, including the presence of morphology, functional groups, crystalline properties, magnetism and thermal stability. Studies have shown that γ-Fe2O3@GMA@IM can adsorb FCF in a wide pH range (2–10), with a maximum adsorption capacity of 445 mg/g. The adsorption data were more in line with the pseudo-second-order kinetic model and the Freundlich isotherm. In order to investigate its reusability, this study used 10% NaCl as the desorption solution, and carried out five batches of adsorption–desorption cycles. After five cycles, the adsorption effect was maintained at 98.3%, which showed a good recycling performance.Keywords:magnetic polymer;ionic liquids;adsorption;reusability
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Chaochi Huang,Jinhe Sun,Ciming Wang,Qian Zhang,Mingyong Wang,Pengrui Zhang,Zixuan Xue,Yan Jing,Yongzhong Jia,Fei Shao
Lithium isotopes (6Li and 7Li) play an important role in the nuclear industry. The development of green and efficient separation methods is a top priority for the lithium isotope industry. In this work, an “aqueous solution|ionic liquid–crown ether organic solution|aqueous solution” system was constructed and used for lithium isotope electromigration separation. The influence and synergy of Li+ diffusion, electromigration, and chelation of crown ether on Li+ migration and isotope separation were investigated, discussed, and verified carefully. The separating laws were summarized. The process and mechanisms of lithium isotope separation were explored preliminarily. The presence of crown ether in organic solution and the introduction of electric field can change the migration ratio and lithium isotope enrichment effect of different parts in the system. The synergy of Li+ diffusion, electromigration, and chelation of crown ether can change the behaviors of Li+ migration and isotope separation significantly. What’s more important, the driving forces are not constant but dynamic. The diffusion increased with the increasing concentration gradient among different parts. The chelation decreased with the increasing Li+ concentration in organic solution. The electromigration also changed with the varied chemical speciation of Li+. The results helped in understanding the roles of driving forces more clearly and provided a foundation for developing green and efficient methods for lithium isotope separation.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
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2022
·Vol. 45
·期 4
·749-759
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IF 3.434
Zhang Xiao-guang,Xue Yu,Lu Ze-ping,Xu Hua-jin,Hu Yi
In this study, a series of proline ionic liquids with different lengths of hydrophobic alkyl on the side chain were used to modify the Candida Antarctic lipase B (CALB). The catalytic activity, thermal stability and tolerance to methanol and DMSO of the modified enzyme were all improved simultaneously. The optimum temperature changed from 55 to 60 ℃. The hydrophobicity and anion type of the modifier have important influence on the catalytic performance of CALB. CALB modified by [ProC 12 ][H 2 PO 4 ] has a better effect. Under the optimal conditions, its hydrolysis activity was 3.0 times than that of the native enzyme, the catalytic efficiency Kcat/Km improved 2.8 times in aqueous phase, and the tolerance to organic solvent with strong polarity (50% methanol 2 h) was increased by 6.8 times. Fluorescence spectra and circular dichroism (CD) spectroscopy showed that the introduction of ionic liquids changed the microenvironment near the fluorophores of the enzyme protein, the α-helix decreased and β-sheet increased in the secondary structure of the modified enzymes. The root mean square deviation (RMSD), residue root mean square fluctuation (RMSF), radius of gyration (Rg), and solution accessible surface area (SASA) of [ProC 2 ][Br]-CALB, [ProC 12 ][Br]-CALB and native CALB were obtained for comparison by molecular dynamics simulation. The results of dynamics simulation were in good agreement with enzymology experiment. The introduction of ionic liquids can keep CALB in a better active conformation, and proline ionic liquids with long hydrophobic chains can significantly improve the surface hydrophobicity and overall rigidity of CALB. This research offers a new idea for rapid screening of efficient modifiers and provision of enzymes with high stability and activity for industrial application.
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高影响因子
SOLAR ENERGY
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2021
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IF 5.742
Yin Huang,Hang Zhong,Wenbo Li,Duoling Cao,Ya Xu,Li Wan,Xu Zhang,Xiuhua Zhang,Yuebin Li,Xiaomimg Ren,Zhiguang Guo,Xianbao Wang,Dominik Eder,Shimin Wang
The potential of perovskite solar cells as a representative alternative to silicon-based solar cells has become significant owing to their unparalleled advancement in efficiency. However, the intrinsic instability of perovskite still hinders their large-scale commercial application, particularly of the decomposition of perovskite during device operation. To address this issue, an acetate-ion-functionalized polar ionic liquid, 1-allyl-3-methylimidazolium acetate (AMIMOAc), is used as an additive in MAPbI 3 film. FTIR spectroscopy measurements show that AMIMOAc can anchor the organic cations via hydrogen bonding and enhance the Pb–O interaction in modified MAPbI 3 , leading to a continuous and dense morphology to increase the stability of MAPbI 3 . After optimizing the concentration of AMIMOAc, an additional interfacial modification layer accelerates the electron extraction and transport. By the synergy of both additive engineering and interface modification, the device not only achieves a high efficiency of 15.16%, but also maintains 93% of the initial PCE after 500 h, showing significantly improved stability. These results pave the way to a new strategy to improve efficiency and long-term stability of carbon counter electrode-based PSCs.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Hao Li,Yingwei Li,Ruirui Wang,Sheng Zhong,Ruirui Zhang,Ruixia Liu
Oxygen vacancies (OVs) engineering is essential in the regulation of the structure and properties of the catalysts for selective oxidation. In this work, the strategy of ionic liquid (IL) mediation was successfully developed in constructing the OV-rich defective Co3V2O8 (CVO), exhibiting excellent performance in cyclohexane oxidation. Coupling the prepotency of the heating treatment, ILs constructed optimal [Bmim][Ac]-CVO-700 possesses the highest OV concentration and catalytic activity with 12.7% cyclohexane conversion accompanied by 89.6% KA oil (cyclohexanol and cyclohexanone) selectivity. Experimental investigation reveals that ILs not only regulates the morphology structure as structure-directing agents but also benefits the formation of OVs through coordination with the Co2+ and V5+. The redox cycle between Co3+/Co2+ and V5+/V4+ was accelerated via the constructed OVs, enhancing the activation of substrates and the transfer of electrons. The distinguished performance is attributed to the rich OVs, porous structure, and synergistic effect between the active metals. The structure–activity relationship between OVs concentration and cyclohexane conversion further indicated that OVs facilitate the essential steps for the generation of targeted products. The possible reaction pathway of cyclohexane oxidation over the OV-rich CVO catalyst was also suggested regarding the radical trapping experiment. This design not only presents a facile and effective strategy for constructing OVs using ILs but also provides an in-depth insight into OV-rich mixed metal oxides in selective oxidation.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Hongyong Zhao,Ting Song,Xiaoli Ding,Ruyi Cai,Xiaoyao Tan,Yuzhong Zhang
Membrane technology for O 2 /N 2 separation is a mature industrial unit. Membranes with excellent permeation-separation performance are still one of the critical requirements. The cobalt-based compounds have been well known for their good affinity for O 2 , which can facilitate O 2 transfer and improve the O 2 /N 2 selectivity in membranes. The cobalt-based compounds, moreover, have a magnetic responsive effect, which can lead to a further improvement in O 2 /N 2 separation under a magnetic field. A class of PIM-1 mixed matrix membranes (MMMs), containing cobalt-based ionic liquid (CILs)@polyarylate (aromatic polyester) (PAR) (core-shell) composite nanospheres (CILs@PAR (c-s) CNPs), were prepared. Chemical compositions of CILs@PAR (core-shell) CNPs were determined by Fourier transform infrared spectroscopy (FTIR). Morphologies and structures of CILs@PAR (core-shell) CNPs were observed by transmission electron microscopy (TEM). Gas adsorption properties of CILs@PAR (core-shell) CNPs were tested. Thermal properties of the (CILs@PAR (c-s) CNPs)/PIM MMMs were investigated by simultaneous thermal analysis (TGA-DSC). Gas permeation-separation performances of the (CILs@PAR (c-s) CNPs)/PIM MMMs were also reported. Compared with the original PIM-1 membrane, the (CILs@PAR (c-s) CNPs)/PIM MMMs display higher O 2 /N 2 selectivity because of cobalt-based ionic liquid as O 2 carrier, coupled with a reduction in O 2 permeability. With increasing the content of the CILs@PAR (c-s) CNPs, the O 2 /N 2 selectivity increases, and the O 2 permeability decreases. It is also found that, as a magnetic field on the MMMs, the O 2 /N 2 selectivity further increases; and it increases more, as a higher content of CILs@PAR (c-s) CNPs. Therefore, the (CILs@PAR (c-s) CNPs)/PIM MMMs exhibit excellent O 2 /N 2 selectivity of ∼5 coupled with good O 2 permeability of ∼140 Barrer under a 180 mT magnetic field and show great potential for air separation.
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JOURNAL OF MOLECULAR STRUCTURE
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2026
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IF 4.9
Yunchang Fan,Shuiqing Yang,Jingjing Chen,Han Wang,Zheng Ruan,Haibao Zhu
Pyridinium PILs outperform quaternary ammonium ones for Au(III) adsorption. • Anion–π and H-bonding synergistically enhance Au(III) capture by pyridinium PILs. • Cl – -form PILs show higher Au uptake than Br – -form due to weaker dispersion forces. • PTPB-Cl achieves fast, selective Au recovery from waste CPU leachate. • PTPB-Cl maintains stable performance and structure over 10 adsorption cycles. A series of pyridinium- and quaternary ammonium-based poly(ionic liquid)s (PILs) with chloride (Cl − ) or bromide (Br − ) counter-anions were synthesized and evaluated for the adsorption of AuCl 4 − from aqueous solutions. The adsorption kinetics followed the pseudo-second-order model, and equilibrium data were well described by the Langmuir isotherm, indicating monolayer chemisorption. Pyridinium-based PILs exhibited significantly higher gold uptake than their quaternary ammonium analogues, attributable to the synergistic contribution of anion–π interactions, and C–H···Cl hydrogen bonding. Chloride-form PILs outperformed their bromide counterparts due to the lower polarizability of Cl⁻, which weakens dispersion interactions with the PIL backbone and facilitates anion exchange. The optimized PIL, PTPB-Cl, achieved efficient gold recovery from actual waste CPU leachate with negligible interference from coexisting metal ions. Moreover, PTPB-Cl maintained stable adsorption and desorption efficiencies over ten consecutive cycles, and post-recycling characterizations confirmed its structural integrity and complete gold desorption. Download: Download high-res image (265KB) Download: Download full-size image
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JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Mohammad Gholinejad,Milad Iranpanah,Shirin Karimi,José M. Sansano
In this study, bimetallic RuCu supported on l -cysteine functionalized ionic liquid modified magnetic nanoparticles (Fe 3 O 4 @IL-Cys-RuCu) was successfully synthesized and characterized. This bimetallic nanocatalyst showed excellent activity in the reduction of 2,3, and 4-nitrophenol isomers and organic dyes as well as catalytic degradation of tetracycline (TC) at room temperature in water. Using this catalyst, complete reduction of nitrophenols was achieved within 9–16 min and degradation of organic dyes and tetracycline were accomplished within 7–4 and 30 min, respectively. The superior activity of bimetallic RuCu compared to similar Ru and Cu catalysts was proved and results indicated that the based on type of reaction, bimetallic catalyst was 2–33 times more efficient than the corresponding monometallic catalysts. This catalyst was recovered and recycled up to 14 times without decreasing in the catalytic activity and stability of the reused catalyst was confirmed by TEM, XRD and XPS.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Chunhong Zhang,Jingsong Cui,Wenbo Sui,Yuning Gong,Hao Liu,Yuhui Ao,Lei Shang
This study investigates the synergistic effects of ionic liquid (IL) and nanofillers on the properties of epoxy resin, aiming to address the issues of brittleness commonly associated with commercial epoxy resins. Starting from molecular structural design, a novel ionic liquid containing amino and phenylboronic acid groups is synthesized via a one-step alkylation reaction. The newly synthesized IL is then synergistically combined with cellulose nanofibers (CNFs) to fabricate a series of IL/CNFs epoxy resin composites. The influence of IL/CNFs content on the thermal properties, mechanical performance, glass transition temperature, and transparency of the composite materials is investigated. Compared to pure epoxy resin (EP), the epoxy composite material with 0.5IL-1.0CNFs exhibits a 50.72 % increase in flexural strength, a 126.94 % increase in elongation at break, and a 97.51 % increase in impact strength. In comparison, both the initial and maximum decomposition temperatures increased (T 5% was 374 °C, and T max was 400 °C), showing an increase of 6 °C and 4 °C, respectively. Additionally, the epoxy composite material maintains high transparency, with a relatively high level of transmittance in the visible light range (400 nm-760 nm). The transmittance at T 500nm increases to 86.8 %, and at T400nm it increases to 69.54 % compared to the pure epoxy resin.
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