BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2018
·Vol. 92
·期 3
·578-584
·
IF 3.526
Geng Tao,Duan Shengfu,Jiang Yajie,Ju Hongbin,Wang Yakui
In this paper, three new kinds of phosphonium-based room temperature ionic liquids (ILs) [Ph3PCH3][CH3(CH2)8COO] (MTPP-D), [Ph3PCH3][CH3(CH2)10COO] (MTPP-L), and [Ph3PCH3][CH3(CH2)12COO] (MTPP-M) were synthesized using triphenylphosphine, dimethyl carbonate and carboxylic acids as raw materials. The viscosity, electrical conductivity, density and surface tension of the synthesized ILs were measured in the temperature range from 298.15 K to 333.15 K under ambient pressure. Meanwhile, the effects of temperature and alkyl chain length on their viscosity, electrical conductivity, density and surface tension were also investigated. The molecular volume, standard entropy, lattice energy and isobaric expansivity of the three ILs were calculated at 298.15 K. Experimental results indicate that the viscosity, density and surface tension of the three ILs decrease significantly with the increase of temperature, while the electrical conductivity shows an opposite trend. The longer the alkyl chain, the higher the viscosity, the lower the electrical conductivity, density and surface tension of the ILs. The experimental dynamic viscosity can be well correlated by the Vogel-Fulcher-Tammann (VFT) equation and simple linear equation. The temperature dependence of electrical conductivity can be well fitted by Arrhenius equation and VFT equation. The molecular volume, standard entropy and isobaric expansivity increase with increasing alkyl chain length, while the lattice energy decreases.
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GREEN CHEMISTRY
·
2026
·
IF 10.6
Yangyang Jiang,Yuxin Liu,Yuanli Qi,Yurou Shao,Dong Wang,Benshuai Guo,Jingyan Zhao,Zhibin Zhou,Yuntao Lei,Lili Jin
The capture and utilization of carbon dioxide (CO2) from the post-combustion of fossil fuels has been identified as a highly effective strategy for reducing carbon emissions. Herein, a series of novel substituted benzenesulfonamide ionic liquids (BSA-ILs) were designed and synthesized via facile acid–base neutralization reactions for the purpose of achieving reversible CO2 capture and catalyzing CO2 chemical fixation. Addressing the inherently high viscosity of neat BSA-ILs (551.2–7785.7 mPa s), propylene carbonate (PC), a green product derived from CO2 chemical fixation, was selected as a diluent to form BSA-IL mixed absorbents (BSA-IL-MAs). The optimized system exhibited a high CO2 uptake capacity of 1.38 mol of CO2 per mol BSA-IL, an excellent CO2/N2 selectivity of 18.36, and a remarkable 99.0% conversion of epichlorohydrin under mild, solvent-free, metal-free, halogen-free, co-catalyst-free and atmospheric pressure conditions. Meanwhile, the findings demonstrated a certain positive correlation between the CO2 uptake capacity/conversion and the pKa of the substituted BSA. Notably, the BSA-IL system retained nearly intact CO2 capture performance and catalytic activity after five consecutive absorption–desorption and catalytic cycles, with an extremely low E-factor of 0.11. Spectroscopic characterization confirmed the formation of a new carbonyl moiety peak in CO2-saturated BSA-ILs, indicating that chemisorption dominated the CO2 uptake process. NMR investigations and DFT calculations further elucidated the interactions between BSA-ILs, CO2 and epoxide substrates, validating the feasibility of the proposed reaction pathways. This work provides a sustainable, efficient and industrially feasible integrated platform for CO2 capture and utilization, offering a paradigm for low-carbon catalytic conversion systems.
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AICHE JOURNAL
·
2026
·
IF 4.4
Yajuan Qu,Xiaoxuan Chen,Haifeng Cong,Xingang Li
The separation of toluene (TOL) and methylcyclohexane (MCH) is a key step to achieve high-purity aromatic recovery, but traditional distillation processes consume significant energy. In this study, an ionic liquids (ILs)-based extractive distillation strategy was proposed to achieve efficient separation by computational screening, experimental validation, and process simulation. First, 1722 candidate ILs were systematically screened using the COSMO-RS model, selecting three high-performance ILs based on selectivity and viscosity criteria. Experimentally determined vapor–liquid equilibrium data showed that 1,3-dimethylimidazolium bis(fluorosulfonyl)imide salt ([MMIM][FSI]) significantly enhanced the relative volatility of TOL-to-MCH. Quantum chemical analyses revealed the separation mechanism. Based on this, an extractive distillation process was constructed by Aspen Plus process simulation: the use of [MMIM][FSI] as an entraining agent reduced the total annualized cost (TAC) by 55.55% compared with conventional distillation. This study provides an industrially feasible solution for low-carbon separation of aromatic/non-aromatic systems through an innovative pathway of molecular design–experimental validation–process integration.
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Green Chemical Engineering
·
2026
·
IF 11.9
Ningjing Tang,Zhen Xu,Youbing Zhu,Ketao Shi,Hui Wang,Tao Zhang
Fluorinated anion-based ionic liquid enables synthesis of ZSM-5 with high framework Al. • Controlled release of F – via anion decomposition promoted framework Al incorporation. • In situ phosphorus modification could stabilize framework Al species. • P-modified ZSM-5 facilitates n -hexane cracking for light olefin production. Direct synthesis of aluminosilicate zeolites with good acidity via fluoride route remains challenging, since such systems generally favor high-silica frameworks and often restrict the incorporation of framework Al. To address this issue, a sustainable strategy for synthesizing aluminosilicate zeolites using hexafluorophosphate ([PF 6 ] – )-based ionic liquid as both structure-directing agent (SDA) and fluorine source (the mineralizing agent) was proposed. This approach enables the fabrication of MFI-, TON-, or ANA-type zeolites under solvent-free and vapor-assisted conditions. Mechanistic investigations using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), solid-state nuclear magnetic resonance (NMR), and two-dimensional (2D) correlation techniques reveal that [PF 6 ] – anions undergo in situ decomposition to release F – in a slow and controlled manner during crystallization. This controlled fluoride-release behavior regulates fluoride availability in the synthesis medium, which facilitated the incorporation of both silicon and aluminum into the zeolite framework, affording ZSM-5 zeolites with lower Si/Al ratios than those obtained using conventional fluoride sources as the mineralizing agent. Simultaneously, phosphorus species generated from [PF 6 ] – were uniformly dispersed within the ZSM-5 zeolite. These in situ -formed phosphorus species could interact with framework aluminum to create stabilizing P-O-Al linkages upon calcination, thereby reducing dealumination and enhancing zeolite acidity when the P content was appropriate. ZSM-5 with retained phosphorus species exhibited superior catalytic performance in n -hexane cracking, achieving high conversion and light olefins yield. This strategy based on multi-functional ionic liquid offers an alternative route to tailor zeolite framework and acid sites for catalytic applications. Download: Download high-res image (216KB) Download: Download full-size image
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Wang Zhao,Cheng Xu,Nuo Xu,Guitao Du,Xiangli Gao,Jianbo Shuai,Zepeng Lei,Xiaohui Wang
With the increasing global demand for sustainable polymers, scalable routes that convert cellulosic feedstocks into high-performance materials are urgently needed. However, efficient dissolution and regeneration of cellulose (CEL) without sacrificing its native degree of polymerization (DP) remain a central challenge in the processing of cellulosic materials. Here, we introduce a hydrophobic-engineered amphiphilic ionic-liquids (AILs) platform that meets this goal. A homologous series of AILs was synthesized by grafting n-alkyl chains of tunable length onto a superbase cation. The resulting AILs dissolve CEL up to 5 times faster than state-of-the-art imidazolium ionic liquids while preserving DP values close to those of the native polymer. Long-time scale (300 ns) molecular-dynamics simulations reveal that the hydrophobic tail of the cation blankets glycosidic linkages against chain scission, whereas the ionic component disrupts inter- and intrachain hydrogen bonds to promote dissolution. This gentle and efficient processing method lowers energy demand and chemical waste, thereby reducing the environmental footprint of biobased material production. By leveraging designable, recyclable AILs, it adheres to green-chemistry principles and supports a circular materials economy. These findings reveal that the amphiphilicity tuning of ionic liquids could be applied as a practical design principle for gentle and efficient processing of sustainable biobased materials.
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ACS Omega
·
2023
·
IF 4.1
Yimei Tang,Kuan Yang,Siyu Zhao,Qingqing Chen,Lan Qin,Bei Qin
To solve the problems associated with poorly water-soluble nonsteroidal anti-inflammatory drugs (NSAIDs), naproxen-based ionic liquids (ILs) containing naproxen as an active pharmaceutical ingredient (API) anion were prepared with benzalkonium (tetradecyldimethylbenzyl ammonium), choline, and 1-octyl-3-methylimidazole as the cation. The structures and thermal properties were analyzed. Through the conductivity method, the solubility at 25 and 37 °C and the critical micelle concentration (CMC) at 25 °C were determined in water and ethanol. The octanol–water partition coefficients (Kow) at 25 °C were measured with the shake-flask method. The cytotoxicity was evaluated with the MTT method. The results showed that the conversion of naproxen into the API-ILs increased the API’s solubility in water by more than 850 times compared with the original API, and the thermostability was satisfactory with a lower glass transition temperature (tg). Moreover, the variation trends of solubility, hydrophilicity, and Kow were consistent with the different structures of naproxen-based ILs, except for benzalkonium naproxen. The CMC (10–5–10–6 M) in water and ethanol demonstrated that the naproxen-based ILs were surface activite ILs. The IC50 values exhibited the low cytotoxicity of the naproxen-based ILs, which was better than 100 μM. The results provide essential information and a research basis for future topical and transdermal administration and oral administration of naproxen-based ILs.
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PubMed
高影响因子
IONICS
·
2023
·Vol. 29
·期 6
·2249-2259
·
IF 2.8
Liu Jie,Xu Yao,Xu Fei,Li Jing,Chen Yanbo,Qiao Junjie,Han Yuyang,Ren Yurong,Lin Bencai
In this study, zwitterionic poly(ionic liquid)-based polymer electrolytes with a network structure are prepared by ultraviolet-irradiation radical polymerization of poly(ethylene glycol) methyl ether acrylate (PEGMEA) and zwitterionic liquids, and poly(ethylene glycol) diacrylate is used as cross-linker. The cross-linked structure endows the electrolytes with high thermal stability and excellent dimensional stability. The abundant ether-oxygen group of PEGMEA provides sufficient sites for the transport of Li + and a high ionic conductivity of 0.20 × 10 −3 S cm −1 . The electrolyte shows a high lithium-ion transference number of 0.78, owing to the excellent dissociation ability of zwitterionic liquids towards lithium salts. The lithium symmetric battery can maintain a voltage polarization of 150 mV at 0.1 mA cm −2 over 600 h. The Li/LiFePO 4 battery shows a discharge capacity of 122 mAh g −1 , a capacity retention of 90.0% after 100 cycles, and an average Coulombic efficiency exceeding 99% at 0.1 C, demonstrating strong application potential in lithium-ion batteries.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2023
·
IF 3.9
Xinwei Mu,Liuxing She,Zaikun Wu,Lidan Deng,Jian kong,Tielin Wang,Yuanhang Qin,Yin Zheng
The SBA-15 molecular sieve carrier with large specific surface area and pore volume, high temperature resistance and acid and alkali resistance was successfully synthesized by the method of hydrothermal synthesis . Then, ionic liquid is loaded on the surface and pores of the carrier by the impregnation method, so that it can be combined with the acid-base COS, thereby enhancing the adsorption effect and adsorption selectivity. Effects of three ionic liquids: 1-ethyl-3-methylimidazolium glycinate, 1-butyl-3-methylimidazolium glycinate and 1–(2-Aminoethyl)3-methylimidazolium bromide on the COS adsorption properties were discussed at different adsorption temperatures and loading concentrations. Among these mesoporous molecular sieves immobilized ionic liquids, the result from COS adsorption shows that the specific surface area of SBA-15 molecular sieve impregnated with 0.9 g·mL −1 [C 2 mim][Gly] (SBA-15-C 2 9.0) decreased from 902 m 2 ·g −1 to SBA-15–27 m 2 ·g −1 . And its COS breakthrough adsorption capacity can reach 11.38 mg·g −1 . It can concluded that [C 2 mim][Gly] is helpful to increase the adsorption capacity.
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RSC Advances
·
2023
·Vol. 13
·期 23
·15762-15771
·
IF 3.9
Zheng Bo,Xu Zhang,Zhesong Huang,Yuhui Huang,Jianhua Yan,Kefa Cen,Huachao Yang
Supercapacitors with high energy and power densities have become highly desirable in practical applications. Ionic liquids (ILs) are considered as promising electrolytes of supercapacitors owing to their excellent electrochemical stability window (approx. 4–6 V) and good thermal stability. However, the high viscosity (up to 102 mPa s) and low electric conductivity (<10 mS cm−1) at room-temperature extremely reduce the ion diffusion dynamics in the energy storage process, resulting in the unsatisfactory power density and rate performance of supercapacitors. Herein we propose a novel binary ionic liquids (BILs) hybrid electrolyte composed of two kinds of ILs in an organic solvent. Along with the organic solvent with high dielectric constant and low viscosity, the addition of binary cations effectively improves the electric conductivity and reduces the viscosity of IL electrolytes. By mixing trimethyl propylammonium bis(trifluoromethanesulfonyl)imide ([TMPA][TFSI]) and N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide ([Pyr14][TFSI]) with an equal mole ratio in acetonitrile (1 M), the as-prepared BILs electrolyte shows superior electric conductivity (44.3 mS cm−1), low viscosity (0.692 mPa s), and a wide electrochemical stability window (4.82 V). The supercapacitors assembled with activated carbon electrodes (commercial mass loading) and this BILs electrolyte achieve a high working voltage of 3.1 V, leading to a maximum energy density of 28.3 W h kg−1 at 803.35 W kg−1 and a maximum power density of 32.16 kW kg−1 at 21.17 W h kg−1, which are obviously superior to those of commercial supercapacitors based on organic electrolytes (2.7 V).
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Dan Chen,Zhe Zhao,Yingying Wu,Sangeeta Prakash,Jie Wan
The dissolution behaviour of three corn starches, including corn starch (CS), high amylose corn starch (HACS) and waxy corn starch (WCS) with different amylose content in 1-allyl-3-methylimidazolium chloride ([AMIM]Cl) and 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) were studied by comparing their dissolution state in ionic liquids (ILs). Further, the structural and thermal properties of the regenerated starch were analyzed. WCS with the lowest amylose content had the fastest dissolution rate, the most extensive structural damage, and the lowest solubility and required the maximum energy for dissolution. In the process of dissolution-regeneration, the A-type crystalline structure of WCS and CS was completely destroyed and transformed into an amorphous structure, while the B-type crystalline structure of HACS transformed into an ordered V -shaped structure. And the thermal stability of starch was improved after dissolution-regeneration in ILs. Among the two kinds of ILs, [AMIM] Cl had a better ability to dissolve starch, causing minor damage to the starch.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Meisi Chen,Mengjia Li,Lin Zhang,Xiemin Liu,Feng Zhang,Youting Wu
Amino acid ionic liquids (AAILs) exhibit prominent merits for CO2 capture including biocompatibility and good stability, but they still suffer from several demerits, such as high viscosity and low molecular utilization. Therefore, it is critical to construct proper systems that can address these problems to enhance CO2 absorption of AAILs. In this work, three types of AAIL absorbent systems, DMEE (2-[2-(dimethylamino) ethoxy] ethanol)–AAIL, H2O–AAIL, and EG (ethylene glycol)–AAIL, are prepared with six AAILs that have different amino acids. The absorption performance of these absorbents is characterized to investigate the reinforcing effects of the additives on the absorption properties of AAILs. With temperatures ranging from 293 to 313 K, the CO2 capture studies on the binary systems reveal that AAILs present better absorption efficiency when their concentrations are 40 or 50 wt %. Based on the zwitterion reaction mechanism model and a thermodynamic model, the interactions of AAILs with H2O, DMEE, and EG systems for absorbing CO2 are discussed, respectively. The results obtained in this work indicate that AAIL–DMEE systems are promising candidates for CO2 capture since the interaction between AAILs and DMEE increases the capacity of AAILs and promotes kinetics.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaoqing Yuan,Ju Liu,Yanlei Wang,Xingming Jie,Jingyu Qin,Hongyan He
Knoevenagel condensation reaction is important for generating C C double bonds and providing various valuable intermediates in organic chemistry, which always need harsh conditions including high reaction temperature, difficult catalyst recovery, difficult product separation, etc. In this work, a novel class of dual-responsive emulsion reactor was prepared for the Knoevenagel condensation reaction between malononitrile and aromatic aldehyde, where the temperature and CO 2 -responsive ionic liquids (ILs) were used as an emulsifier, responder, and catalyst simultaneously. Driven by temperature or CO 2 , the emulsion reactor undergoes reversible and controllable transformations between emulsification and demulsification, where efficient catalytic reactions, product separation, and reactor recovery are all achieved. The isolated product yield of 2-(4-chlorobenzylidene)-malononitrile remained above 90% after 5 cycles of the emulsion reactor. NMR and molecular dynamics simulations showed that the temperature drives the reversible stretching and curling of the polyether chain on the cation, while CO 2 reacts with the –COO - group on the anion to form carbonates and carboxylic acids in water, leading to changes in the surface activity of ILs, thereby reversibly regulating the demulsification and emulsification of the emulsion. Hence, through the dual stimuli-responsive ILs, the efficient reaction can be performed in the homogeneous phase, and the products and catalysts can be easily separated in the heterogeneous phase. These results on the revisable microreactor can not only help to design the smart and efficient “homogeneous reaction-heterogeneous separation” systems but also support the development of green sustainable chemistry.
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危险品化学品经营许可证（带存储）