Journal of CO2 Utilization
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2021
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IF 7.132
Ye Qu,Yanglin Chen,Jianmin Sun
CO 2 utilization plays an important role in rational use of carbon resources and reduction of carbon emissions. It is still a challenge to achieve efficient CO 2 utilization by amino acid ionic liquids (AAILs) under room temperature and atmospheric pressure with cocatalyst- and solvent-free conditions. Herein, the newly developed AAILs including 1,1,3,3-tetramethylguanidine cation ([HTMG] + ) together with both amino acid and halogen as anions, were simply synthesized by neutralization reaction. Under mild conditions (30 °C, 20 h and 1 MPa CO 2 ), the cycloaddition reaction of CO 2 and propylene oxide could be efficiently catalyzed by [HTMG][His][I] with 99 % propylene carbonate yield and selectivity in the absence of additional solvent and cocatalyst. Notably, even at room temperature and atmospheric pressure for 72 h, [HTMG][His][I] also displayed 96 % yield and 99 % selectivity due to the cooperation of [HTMG] + , [His] 2– and [I] – . Meanwhile, [HTMG][His][I] performed excellent universality of various epoxides and reusability. Based on the characterization results of 1 H and 13 C NMR, it was verified that propylene oxide and CO 2 were simultaneously activated by the functional groups in [HTMG][His][I]. Hence, the reaction mechanism for CO 2 cycloaddition with epoxide catalyzed by [HTMG][His][I] was proposed. This work provided a simple strategy to prepare sustainable AAILs for efficient CO 2 utilization under very mild conditions of room temperature and atmospheric pressure (even the low CO 2 concentration at simulated flue gases).
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Li Zhang,Weiwei Lu,Peng Xu,Hao Wang,Xuefeng Wei,Kaisheng Yao,Shuge Peng
In this study, we propose a novel photo-activation method to remove persistent organic pollutants through a SO4˙ˉ-based advanced oxidation process . Core–shell Ag@Pd nanocubes were prepared by a facile seed-mediated method and, afterward, explored for photodegradation of a representative ionic liquid (IL), [C 4 mim]Br. Electron paramagnetic resonance measurements and radical scavenging experiments demonstrated that the species mainly responsible for degrading [C 4 mim]Br were the radicals of SO4˙ˉ. The plasmon-mediated nature of the Ag@Pd catalysts was verified by their wavelength-dependent performance. Subsequent optical simulation indicated that, other than the plasmonic Ag core, the non-plasmonic Pd shell was the preferential site for dissipating the absorbed photons into energetic charge carriers to produce the radical species. Finally, based on the detected intermediates, we propose the degradation pathway of ILs in the plasmon-mediated process. The results of our method suggest favorable application in the treatment of wastewater.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Yipeng Zheng,Zhennan Cao,Zheng Zhou,Gaodong Yang,Zhibing Zhang
A series of SO 3 -functional Brønsted acidic ionic liquids (SBAILs) were prepared to catalyze the N -formylation of aniline with DMF . The reaction conditions such as ionic liquid type, reaction temperature, catalyst loading and molar ratio of reactants were investigated. To the best of our knowledge, kinetic model for the N -formylation of aniline with DMF using SBAIL was firstly built and simulated. The studies on the reaction order of the reaction were evaluated by initial concentration method, and the kinetic parameters such as reaction rate constant and activation energy were proposed and used to explain the catalytic activities of the SBAILs catalysts. Accordingly, the recycling experiments showed that the SBAIL [Bsmim][HSO 4 ] can be easily recovered and reused with stable activity. Further, the temperature-controlled study emphasized that the ionic liquid was easy to be separated and environmentally friendly.
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EUROPEAN POLYMER JOURNAL
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2021
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IF 4.598
Qiaohong Peng,Li Wei,Xiaoyan Zhang,Ying Wu,Khalid Mahmood,Zhengping Liu,Lisha Zhang
Ionic liquids (ILs), instead of the classical organic solvents, have shown great improvements in chemical processes. Herein, Water-insoluble alkyl- and benzyl-substituted imidazolium bis(trifluoromethanesulfonyl)imides as non-volatile and thermostable solvents were employed in the direct polycondensation of l -lactic acid (LLA). The effects of monomer concentration, reaction temperature and miscibility between the ILs and poly( l -lactic acid) (PLLA) were comprehensively investigated. Biodegradable PLLA with weight-average molecular weight as high as 132 kDa was synthesized. Compared to melt-polycondensation of LLA, far higher molecular weight could be achieved via the solution polycondensation of LLA in ILs since the viscosity of the polymer melt could be significantly reduced based on the dilution effect of ILs. Polycondensation kinetics of LLA in bulk and in an IL demonstrated that the IL could accelerate the polycondensation of LLA. Influence of lactide, the main by-product, on the polycondensations of LLA was also studied kinetically.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Ke Wang,Yuxia Liu,Shiting Wang,Zhifeng Dai,Yubing Xiong
Synergistic effect between different functional groups is of significant influence on the activity of catalysts, especially for bi- or multi-component catalysts. Herein, a binary catalyst composing of metalloporphyrin (MPP) and phosphonium ionic liquid (PIL) is developed. The influence of substitution groups in both MPP and PIL on the cycloaddition addition of carbon dioxide and epoxides was comprehensively studied. The results demonstrated that the introduction of both electron-donating and electron-withdrawing functional groups in 5,10,15,20-tetraphenylporphyrin (TPP) framework was unfavorable to CO 2 transformation. Moreover, PIL cocatalyst with longer alkyl group could enhance the catalytic activity obviously. When Co 3+ was used as the metal active center, the binary catalyst system (TPP/Ph 3 PHexBr) could endow cyclic carbonate with a quantitative yield under the ambient condition of 50 °C and 1 atm CO 2 pressure. The turnover frequency (TOF) value could also be as high as 191.3 h –1 . Our founding thus provides an insight into the design of binary catalysts for efficient transformation of CO 2 .
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Qingxiang Liu,Tao Zhang,Peng Gao,Jun Gao,Dongmei Xu,Pingping Zhao,Lianzheng Zhang,Yinglong Wang
As a hopeful solvent, ionic liquids with tremendous combination of functional chemical sites in the cations and anions can make the separation process efficiently and selectively. Thus, to test the effect of the functional chemical sites in the cations and anions on extracting typical heterocyclic N -compound, indole was adopted as the representative compounds due to its high content and valuable application. In present work, NMP-based IL, [EtOHpyr][BuRA], with dual functional chemical sites was designed and employed to separate indole from diverse resources. The mechanism for the separation process was explored, the IL is evaluated to separate indole with the polarity analysis based on the COSMO-SAC model. Molecular dynamics simulation analysis contributed to understand the H-bonds interaction between indole and IL more indicative. The results demonstrated that the H-bonds between indole and dual functional chemical sites in [EtOHpyr][BuRA] served as the key driving force during the separation process. To validate the effect of functional chemical sites, [EtOHpyr][BF 4 ], [Etpyr][BuRA] and [Etpyr][BF 4 ] were also used for comparison. Furthermore, the influence of extraction of NMP-based ILs on indole, mass ratio (IL: model oil) and extraction temperature were investigated. Under the optimal conditions (25 ℃, mass ratio = 1:5), [EtOHpyr][BuRA] showed the best performance among those four ILs, which extraction efficiency can reach up to 95.15 wt%. The results agreed with the simulation results well. This work can provide an efficient designed ILs for the extraction of indole.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Shahid Hussain,Haifeng Dong,Shaojuan Zeng,Muhammad Umair Ahmad,Farooq Khurum Shehzad,Hui Wu,Yanqiang Zhang
Ionic liquids, which are designable and nonvolatile, have become a hot topic in the field of CO 2 separation from industrial gases. In order to utilize the nonvolatile and low heat capacity of ionic liquids, it is necessary to solve the problem of high viscosity of pure ionic liquids. In the present study, ether functionalized pyridinium ion [E 1 Py] + with good biodegradability and low viscosity was selected as cation. Ions containing cyano groups were used as anions, such as thiocyanate ion [SCN] - , dicyanamide ion [N(CN) 2 ] - , tricyanomethanide ion [C(CN) 3 ] - . Three ionic liquids with low viscosity were synthesized and characterized by 1 HNMR, 13 CNMR and FTIR. The physiochemical properties of ionic liquids such thermal decomposition temperature, density and viscosity were tested. The CO 2 absorption capacity was systematically studied by using intelligent gravimetric analyzer at the pressure range between 0 and 15 bars and the temperature range from 303.15 to 333.15 K. The results showed that the order of CO 2 absorption capacity of these three ionic liquids is [E 1 Py][C(CN) 3 ] > [E 1 Py] [N(CN) 2 ] > [E 1 Py][SCN], which showed that the solubility increased by increasing more cyano groups in ionic liquids. Thermodynamic properties such as enthalpy, entropy, and Gibbs free energy were also calculated for CO 2 absorption.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Shengxin Chen,Ran An,Yingwei Li,Yuting Zhu,Xinbao Zhu,Ruixia Liu,Xingang Li,Suojiang Zhang
In recent years, multi-ionic liquids (ILs) mixture systems have been widely noticed and applied in catalysis due to their unique properties. In order to establish the quantitative relationship between parameters and catalytic behavior, double salt ILs (DSILs), with different cation (1-ethyl-3-methylimidazolium, choline, tetraethylammonium) but same anion (acetate), are performed in the coupling reaction of propylene oxide (PO) with methanol. In the present work, the DSILs properties like Hammett basicity (H0), hydrogen bond donor (HBD) ability (α), hydrogen bond acceptor (HBA) ability (β) and dipolarity/polarizability effect (π*) were considered in the reaction. These control factors were quantitative related to catalytic performance by a modified liner solvent energy relationship (LSER) function that adding a Hammett function correction term. According to the modified-LSER, solvents with different parameters were tested to verify its validity and control the reaction. This study demonstrated each parameter could make a different contribution to chemical reaction. It provides a new perspective way for multi-ILs mixture avoiding the intricacies of the parameter relation in ILs catalysis reasonably.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Kehui Hu,Mengke Kong,Mengyi Qin,Jinchao Zeng,Bin Ai,Jiayi Zhang,Huiwen Zhang,Fei Zhong,Guowei Wang,Linghua Zhuang
Typical hydrogen bonding information (hydrogen bonds, hydrogen bond lengths, and average bond lengths) and weak interaction energy (ΔH) of four ionic liquids (ILs), anion/chitobiose, cation/chitobiose, and IL/chitobiose complexes were determined using density functional theory (DFT) calculations to elucidate the contribution ratio effect of ions (cations or anions of ILs) upon chitosan dissolution. For [Emim]Ac and [Bmim]Ac with same acetate anion, contribution ratio (Rc) values of cations in [Bmim]Ac and [Emim]Ac increased from 37.88% to 38.14%. For [Bmim]Cl and [Etmim]Cl with same chloride anion, contribution ratio (Rc) values of cations increased slightly from 39.39% to 41.65%. As for [Bmim]Cl and [Bmim]Ac with same cation, contribution ratio (Rc) values of Cl- anion in [Bmim]Cl (60.61%) was lower than that of acetate anion in [Bmim]Ac (62.12%). These changes revealed that cations of ILs played more important role in chitosan dissolution. Hydrogen-bond basicity values (β values) of ILs were closely related to the DFT simulation results (weak interaction energy and average hydrogen bond length values) of ILs. Chitosan dissolved faster in acetate based imidazolium ILs ([Emim]Ac and [Bmim]Ac) than the chloride based ILs ([Bmim]Cl and [Etmim]Cl). The chitosan dissolution performance in ILs was consistent with DFT simulation results (weak interaction energy values and average hydrogen bond length values) of IL/chitobiose and hydrogen-bond basicity values of ILs.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2020
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IF 2.369
Jin Liu,Xiaochen Qi,Li Li,Ning Chang,Jie Wei,Dawei Fang,Zhiheng Zhang
The binary mixtures composed of 1-ethyl-3-(2-methoxyethyl)-imidazolium bis(trifluoromethylsulfonyl)imide [C22O1IM][NTF2] and alcohols were prepared, and the density and viscosity were measured first across the entire range of mole fraction within a particular temperature range. Based on the experimental values of density, the average molar volume, the excess molar volume, and the partial molar volume were calculated, and the excess molar volume was well fitted by Redlich–Kister equation. In addition, in order to describe the excess activation Gibbs energy of viscous flow simply and directly, the relative volume of mixtures, Vr, is introduced in this paper and then combined with the relative viscosity, ηr, and a new find about the nondimensional Gibbs energy of activation for viscous flow of the mixture, ΔG⧧E/RT, could be obtained.
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ACS Omega
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2020
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IF 2.87
Qin Wu,Quan Shi,Jiqing Shang,Min Wang,Hansheng Li,Daxin Shi,Yun Zhao,Qingze Jiao
Surface-active heteropolyacid-based ionic liquids with varying alkyl carbon chains were synthesized, which were subsequently analyzed. The desulfurization of fuels was investigated utilizing various surface-active heteropolyacid-based ionic liquids, and acetonitrile was used as the extractant for the coupling of ODS and EDS. The influences of the alkyl group, surface activity, and hydrophobicity of ionic liquids on sulfur removal were studied. The results suggested that the ionic liquids were stable. Among these ionic liquids, [C4ImBS]3[PW12O40] exhibited the best catalytic performance. Using [C4ImBS]3[PW12O40] as the catalyst, the influences of the catalyst amount, aqueous hydrogen peroxide amount, and reaction temperature on the sulfur removal were explored. Under the optimum conditions, the sulfur removal could achieve 100% efficiency. The recycle experiments also proved that the ionic liquid could be reused.
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PubMed
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RSC Advances
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2020
·Vol. 11
·期 2
·700-710
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IF 3.119
Shurong Gao,Jiaxin Jin,Masroor Abro,Ruozhen Song,Miao He,Xiaochun Chen
Extractive denitrification (EDN) of shale oil using ionic liquids (ILs) as the extracting agent has good industrial prospects. In such processes, ILs with higher selectivity to N-compounds and lower solubility in shale oil are desired to improve the EDN efficiency, and reduce the loss of ILs and the contamination of shale oil. In the present study, we employed COSMO-RS to calculate the selectivity of 70 ILs to the typical N-compounds (pyridine, quinoline and indole). The influence of the IL structural characteristics, composition of shale oil and properties of N-compounds are investigated from a micro-level view with the σ-surface and σ-profile. The selectivity strongly depends on anionic species and it is greatly influenced by hydrogen bonding (HB) and π–π interaction between N-compounds and ILs. ILs composed of [H2PO4]− and [MeSO3]− with larger HB donor energy show higher selectivity to the basic N-compounds, while ILs composed of [Ac]− with larger π-electron cloud density show higher selectivity to the non-basic N-compounds. Anions with stronger polarity have lower solubility in shale oil. Moreover, experimental determinations of EDN indicated that [C4py][H2PO4]/[C4mim][H2PO4] and [C2mim][Ac]/[C2py][Ac] have good EDN performance for quinoline/pyridine with efficiency of 100% and for indole with efficiency of 91%, respectively. This work presents a theoretical basis to design and select ILs having higher selectivity for N-compounds and lower solubility in shale oil for use in denitrification.
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