ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Weida Chen,Meisi Chen,Tong Lei,Feng Zhang,Jiao Geng
High regeneration energy is a critical barrier to the large-scale implementation of CO2 capture technologies. To address this challenge, we present a novel energy-efficient biphasic absorbent system, designed by incorporating sterically hindered amine ionic liquids (AMP-TZ) with N,N,N′,N′-tetramethyl-1,6-hexanediamine (TMHDA). The innovative design focuses on enhancing the spatial site resistivity of ionic liquids, which plays a key role in optimizing the CO2 absorption and minimizing regeneration energy. This system demonstrates superior performance, achieving a CO2 absorption capacity of 2.72 mol/kg at 313.2 K and 150 kPa, with a low regeneration energy of 2.31 GJ/t of CO2. Molecular dynamics simulations and quantum chemical calculations reveal that AMP-TZ promotes proton transfer during absorption and stabilizes bicarbonate (HCO3–) in the CO2-rich phase via weak hydrogen bonding. The unique role of AMP-TZ as a bifunctional hydrogen bond donor/acceptor and its ability to suppress the self-aggregation of HCO3– enhance both the absorption efficiency and regeneration performance. This study provides insights into the design of low-hydration CO2 capture systems and offers a theoretical framework for developing highly efficient, energy-saving biphasic absorbents.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Sibo Qiao,Lulu Dong,Yifan Jia,Yinghao Zhang,Lixia Bao,Yiyang Kang,Yufei Wang,Weichao Lin,Pengpeng Liu,Jiliang Wang
Interactions between polysaccharides and ionic liquids (ILs) at the molecular level are essential to elucidate the dissolution and/or plasticization mechanism of polysaccharides. Herein, saccharide-based ILs (SILs) were synthesized, and cellulose membrane was soaked in different SILs to evaluate the interactions between SILs and cellulose macromolecules . The relevant results showed that the addition of SILs into cellulose can effectively reduce the intra- and/or inter-molecular hydrogen bonds of polysaccharides. Glucose-based IL showed the intensest supramolecular interactions with cellulose macromolecules compared to sucrose- and raffinose-based ILs. Two-dimensional correlation and perturbation-correlation moving window Fourier transform infrared techniques were for the first time used to reveal the dynamic variation of the supramolecular interactions between SILs and cellulose macromolecules. Except for the typical HO⋯H interactions of cellulose itself, stronger –Cl⋯HO hydrogen bonding interactions were detected in the specimen of SILs-modified cellulose membranes. Supramolecular interactions of –Cl⋯H, HO⋯H, C–Cl⋯H, and –C=O⋯H between SILs and cellulose macromolecules sequentially responded to the stimuli of temperature. This work provides a new perspective to understanding the interaction mechanism between polysaccharides and ILs, and an avenue to develop the next-generation ILs for dissolving or thermoplasticizing polysaccharide materials.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 1.6
Ping Xie,Tianhao Zhong,Tao Li,Yiwu Lu,Yingmin Yu,Qingshan Zhao,Zhongtao Li
There is an urgent need to develop green catalytic transesterification technology to reduce liquid waste and instrument corrosion. Ionic liquids with controlled activity, easy recovery, and corrosion resistance have great potential as catalysts for transesterification reactions. In this paper, a series of ionic liquids were prepared using imidazole and ammonium compounds as cations, and sulphuric acid, p -toluenesulfonate, and bistrifluoromethanesulfonate anions as anions. In comparison, the ionic liquid made from imidazole with H 2 SO 4 (IMIHS) was found to be the best catalyst for the esterification reaction with high speed, high activity, low corrosion, and high stability, and its catalytic performance was superior to that of sulphuric acid. The optimum reaction conditions were as follows: the molar ratio of ethanol to acetic acid was 1:1, the catalyst amount was 5 wt.%, the reaction temperature was 80°C, and the reaction time was 120 min. The maximum yield of ethyl acetate was 66.2% under the optimum reaction conditions. The catalytic activity was not declined obviously by reusing six times. The activation energy of the reaction is 48.748 kJ/mol.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hongping Li,Wendi Fu,Jie Yin,Jinrui Zhang,Hongshun Ran,Ming Zhang,Wei Jiang,Wenshuai Zhu,Huaming Li,Sheng Dai
Developing a highly efficient strategy for the stabilization of the solid-liquid interface is a persistent pursuit for researchers. Herein, porous ionic liquids based on UiO-66 (Zr) porous materials were synthesized and applied to the selective desulfurization catalysis, which integrates the permanent pores of porous solids with the exceptional properties of ionic liquids. Results show that porous ionic liquids possess high activity and selectivity for dibenzothiophene. Experimental analysis and density functional theory calculations revealed that the ionic liquids moiety served as an extractant to enrich dibenzothiophene into the porous ionic liquids phase through the π···π and C H···π interactions. Additionally, the electrostatic solvent effect in the porous ionic liquids contributes to the stabilization solid-liquid interface, which was favorable for UiO-66 moiety to catalytically activate hydrogen peroxide (H 2 O 2 ) to generate ·OH radicals, and subsequently oxidized dibenzothiophene to the corresponding sulfone. It is hoped that the development of porous ionic liquids could pave a new route to the stabilization of the solid-liquid interface for catalytic oxidation.
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高影响因子
MOLECULES
·
2017
·Vol. 22
·期 8
·1353
·
IF 2.861
Jianliang Sun,Hao Liu,Wenping Yang,Shicheng Chen,Shiyu Fu
Water-miscible alkylimidazolium ionic liquids (ILs) are “green” co-solvents for laccase catalysis, but generally inhibit enzyme activity. Here, we present novel insights into inhibition mechanisms by a combination of enzyme kinetics analysis and molecular simulation. Alkylimidazolium cations competitively bound to the TICu active pocket in the laccase through hydrophobic interactions. Cations with shorter alkyl chains (C2~C6) entered the channel inside the pocket, exhibiting a high compatibility with laccase (competitive inhibition constant Kic= 3.36~3.83 mM). Under the same conditions, [Omim]Cl (Kic= 2.15 mM) and [Dmim]Cl (Kic= 0.18 mM) with longer alkyl chains bound with Leu296 or Leu297 near the pocket edge and Leu429 around TICu, which resulted in stronger inhibition. Complexation with alkylimidazolium cations shifted the pH optima of laccase to the right by 0.5 unit, and might, thereby, lead to invalidation of the Hofmeister series of anions. EtSO4−showed higher biocompatibility than did Ac−or Cl−, probably due to its binding near the TICu and its hindering the entry of alkylimidazolium cations. In addition, all tested ILs accelerated the scavenging of 2, 2′-azino-bis-(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS) radicals, which, however, did not play a determining role in the inhibition of laccase.Keywords:ionic liquids (ILs);laccase;alkylimidazolium cations;competitive binding;kinetics;Hofmeister effects;molecular simulation
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JOURNAL OF SURFACTANTS AND DETERGENTS
·
2015
·Vol. 18
·期 3
·421-428
·
IF 1.685
Xu Wenwen,Zhang Qian,Wei Hongtu,Qin Jieqiong,Yu Li
The self-aggregation behavior of catanionic surface active ionic liquids (SAIL), 1-alkyl-3-methylimidazolium alkyl sulfates, [C 4 mim][C 16 SO 4 ] and [C 6 mim][C 14 SO 4 ], in aqueous solutions was explored by several techniques. These results were analyzed together with the concerning data of [C 8 mim][C 12 SO 4 ] reported previously. The feature of these SAIL is that the total carbon number of the hydrophobic chains is kept constant, while only the length of the two hydrocarbon chains varies. Because of the different intermolecular and intramolecular interactions, the hydrophobic interaction of asymmetrical SAIL is enhanced, which explains the minimal CMC value of [C 4 mim][C 16 SO 4 ]. Thermal motion of hydrocarbon chains at the air–water interface leads to higher A
min and lower Γ max values with the increasing asymmetry of two hydrophobic chains. The conductivity measurements reveal that the micellization process is spontaneous and entropy-driven in the studied temperature range. This work indicates that the symmetry of alkyl chains can influence the aggregation behavior of [C
n
mim][C
m
SO 4 ] in aqueous solutions.
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POLYMER
·
2014
·
IF 3.766
Heng Zhang,Li Li,Wenfang Feng,Zhibin Zhou,Jin Nie
A new family of polymeric ionic liquids (PILs) based on alkyl and alkyl ether substituted ammoniums and perfluorinated sulfonimides (i.e., bis(fluorosulfonyl)imide (FSI − ), and bis(trifluoromethanesulfonyl)imide (TFSI − )) have been synthesized by polymerization of the corresponding ionic liquid monomers (ILMs). Their structures and compositions have been characterized by 1 H and 19 F NMR, FTIR and viscosity-average molecular weight ( M v ). The physicochemical properties of both the ILMs and the PILs have been studied in terms of thermal stability, phase transition, and ionic conductivity . All the prepared ILMs and PILs reveal excellent thermal stabilities to greater than 250 °C. The PILs containing alkyl ether side unit show significant decrease in glass transition temperature ( T g ), the values of T g of the alkyl ether based-PILs are all significantly lower by 10–77 °C in magnitude than those of the corresponding alkyl based ones. The ionic conductivity of alkyl ether based-PILs in the best case increases up to 4.0 × 10 −6 S cm −1 at 30 °C, and reaches 7.6 × 10 −5 S cm −1 at 60 °C, and outperform their ammonium counterparts with alkyl side chain that were synthesized as references.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
·
IF 2.567
Xuan Zhang,Rui Zhang,Haiyan Liu,Xianghai Meng,Chunming Xu,Zhichang Liu,Peter A. A. Klusener
Pyridine can act as a basic indicator for both Brønsted and Lewis acids forming different types of bonds. Infrared spectroscopy, in combination with 27Al NMR spectroscopy, was employed to study the interaction mechanism of pyridine and chloroaluminate ionic liquids (ILs). The acid type, acid amount, acidity, and even activity of chloroaluminate ILs could be determined. An in situ infrared complexometric titration was developed as a quantitative characterization method for determining the different acidities and catalyst activity. The method is based on the principle that Lewis acidic chloroaluminate [Al2Cl7]− anion reacts with pyridine to form the [AlCl4]− anion and pyridine–AlCl3 ([PyAlCl3]) complexes, while the Brønsted acid forms a pyridinium salt. Both product types showed characteristic shifts of the pyridine peaks in the infrared spectrum.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2015
·
IF 2.037
Fufeng Cai,Wei Zhu,Yanbin Wang,Tongzhen Wang,Guomin Xiao
In this work, the ability of ionic liquids (ILs) 1,3-dimethylimidazolium dimethylphosphate ([MMIM][DMP]), 1-ethyl-3-methylimidazolium diethylphosphate ([EMIM][DEP]), and 1-butyl-3-methylimidazolium dibutylphosphate ([BMIM][DBP]) as alternative solvents used in liquid removal of toluene from its combination with heptane was studied. The liquid–liquid equilibrium (LLE) data in relation to ternary systems {toluene + heptane + [MMIM][DMP], [EMIM][DEP], or [BMIM][DBP]} calibrated at T = 298.2 K and atmospheric pressure. The LLE results studied in relation to ternary systems were fitted by the thermodynamic nonrandom two-liquid (NRTL) model. The toluene solute distribution ratios and toluene/heptane selectivities, derived from the experimental LLE data, were compiled and analyzed to determine the extraction capacity of the studied ILs.
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GREEN CHEMISTRY
·
2016
·Vol. 18
·期 23
·6246-6254
·
IF 8.506
Yan-Rong Liu,Kaj Thomsen,Yi Nie,Suo-Jiang Zhang,Anne S. Meyer
In this work, 357 ionic liquids (ILs) formed from 17 cations and 21 anions were selected for evaluation of their ability to dissolve cellulose by COSMO-RS. In order to evaluate the predictive model and method, experimental measurements of the solubility of microcrystalline cellulose (MCC) in 7 of these ILs were also conducted. Predicted results from logarithmic activity coefficients were generally in good agreement with the experimental results. Three different models were used for describing cellulose, and the mid-monomer part of the cellotriose model was found to be closer to the experimental results than a neat glucose model and the model of the mid-dimer part of cellotetraose. Excess enthalpy calculations indicated that hydrogen-bond (H-bond) interactions between cellulose (i.e. the three cellulose models) and the 7 studied ILs are key factors for the solubility of cellulose, and the anions play a crucial role in the cellulose dissolution process. Importantly, the cations of methylimidazolium+, pyridinium+, ethylmorpholinium+ and methylpyrrolidinium+ structured with functional groups including ethyl, allyl, 2-hydroxylethyl, 2-methoxyethyl and acryloyloxypropyl, combined with anions Ac−, Dec−, HCOO−, Cl−, BEN−, DMPO4−, DEP−, DBP− and Br− were predicted to be the best for dissolving cellulose.
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Chinese Physics B
·
2022
·Vol. 31
·期 3
·037802
·
IF 1.652
Weifeng Ma,Chunjie Ding,Nasrullah Wazir,Xianshuang Wang,Denan Kong,An Li,Bingsuo Zou,Ruibin Liu
The methylammonium lead triiodide (CH3NH3PbI3)-based perovskite shows a great alluring prospect in areas of solar cells, lasers, photodetectors, and light emitting diodes owing to their excellent optical and electrical advantages. However, it is very sensitive to the surrounding oxygen and moisture, which limits its development seriously. It is urgent to spare no effort to enhance its optical and electrical stability for further application. In this paper, we synthesize the MAPbI3 perovskite film on the glass substrate with/without the ionic liquid (IL) of 1-Butyl-3-methylimidazolium tetrafluoroborate (BMIMBF4) by a simple two-step sequential solution method. The additive of BMIMBF4 can improve the quality of crystal structure. Moreover, the photo-luminescence (PL) intensity of MAPbI3 film with BMIMBF4 is much stronger than the pure MAPbI3 film after a week in the air, which is almost ten-fold of the pure one. Meanwhile, under the illumination of 405-nm continuous wave (CW) laser, the fluorescent duration of the MAPbI3 film with BMIMBF4 is approximately 2.75 min, while the pure MAPbI3 film is only about 6 s. In fact, ionic liquid of BMIMBF4 in the perovskite film plays a role of passivation, which prevents the dissolution of MAPbI3 into CH3NH3 and PbI2 and thus enhances the stability of environment. In addition, the ionic liquid of BMIMBF4 possesses high ionic conductivity, which accelerates the electron transport, so it is beneficial for the perovskite film in the areas of solar cells, photodetectors, and lasers. This interesting experiment provides a promising way to develop the perovskite's further application.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Jingli Han,Yuanyuan Fan,Gangqiang Yu,Xuzhao Yang,Yingying Zhang,Junfeng Tian,Guoxuan Li
The ethanol (EtOH) dehydration process using ionic liquids (ILs) as entrainers by extractive distillation integrated with a heat pump was systematically investigated from the molecular level to the process scale. [BMIM][Cl] was selected as the appropriate entrainer from a variety of [Cl]−-based ILs by achieving vapor–liquid equilibrium (VLE) experiments for binary systems of EtOH–IL and water (H2O)–IL. The VLE behavior of a ternary EtOH–H2O–IL system demonstrates that the azeotropic phenomenon of the binary EtOH–H2O system is effectively broken in the presence of IL. Moreover, the UNIFAC model was successfully extended to predict the VLE of the EtOH–H2O–IL system. The microscopic mechanism of the EtOH–H2O separation with [BMIM][Cl] as an entrainer at the molecular level was identified by performing molecular dynamics simulations. It is found that hydrogen bond interactions of EtOH/H2O–[BMIM]+ and −[Cl]− play crucial roles in breaking the azeotropic phenomenon. The equilibrium stage model for the ethanol dehydration process with [BMIM][Cl] as an entrainer was established, wherein the binary group interaction parameters of the UNIFAC model were embedded. The process simulation and optimization were performed at the industrial scale. The extractive distillation process intensified with the heat pump technology has better economic and environmental efficiencies when compared with the conventional one. The total annual cost and CO2 emission of the former are reduced by 27.01 and 80.46%, respectively, compared with those of the latter. In short, the process intensification technology for ethanol dehydration by using ILs as entrainers integrated with the heat pump proposed in this work is in line with sustainable chemical separation processes, which can be directly extended to other extractive distillation processes with ILs.
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