JOURNAL OF CHEMICAL THERMODYNAMICS
·
2021
·
IF 3.178
Yanli Zhang,Huiyuan Li,Haixia Li,Rongli Shan,Zhaoyou Zhu,Yinglong Wang,Jun Gao
Selecting green and efficient extractive solvents are the inevitable requirement of sustainable development. Ionic liquids as green solvents are widely used in the separation of organic substance. In this manuscript, ionic liquids are used as extractive solvents to separate isopropyl ether-acetone system. The selected ionic liquids are 1-ethyl-3-methylimidazole dinitrile amine [EMIM][DCA], n-butyl-3-methylimidazole trifluoromethane sulfonate [BMIM][OTF], 1-ethyl-3-methylimidazole trifluoromethane sulfonate [EMIM][OTF]. Firstly, the relation between H-bonding donor and H-bonding acceptor is description by COSMO-SAC model based on the extraction mechanism. After that the experiments of liquid–liquid equilibrium are conducted at T = 298.15 K and P = 101.325 kPa, and the liquid–liquid equilibrium data are correlated by NRTL model. The results indicate that the model has a good correlation with the experimental results. Finally, the extraction mechanism is discussed at micro scale. The H-bonding interaction between ionic liquids and acetone, including total charge density, bond length, deformation charge density and interaction energy, is determined by quantum chemistry calculation. The quantum chemical calculation and experimental process provide theoretical guidance for the highly efficient separation of acetone - isopropyl ether binary system.
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高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 11
·e18206
·
IF 3.7
Shuyue Wen,Tao Wang,Xiaomin Zhang,Weigao Xu,Xingbang Hu,Youting Wu
This article proposes for the first time the preparation of a series of amino acid ionic liquids (AAILs) via one-step hydrolysis of cheap lactams for the capture of CO 2 . The structures of the prepared AAILs are confirmed using NMR, FTIR, and ESI-MS, and their physical properties are also determined. It is found that these AAILs are reversible CO 2 absorbents with very high absorption capacities (0.15 to 0.18 g·g −1 at 313.2 K and 1.0 bar), better than almost all task-specific ionic liquids reported in literatures. The absorption mechanism is also elucidated to be a combination of 1:1 and 2:1 stoichiometric reaction of AAILs with CO 2 from NMR, FTIR, reaction equilibrium thermodynamical modeling and quantum calculations. The AAILs have the advantages of simple synthesis, high yield, and using available cheap raw materials. It is believed that this kind of AAILs have great potentials to be used as efficient CO 2 absorbents.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Bowen Jiang,Meiling Weng,Jigang An,Yuewei Fan,Jia Liu,Ying Liu,Ting Yu,Leizhi zheng,Guoqiang Yang,Zhibing Zhang
The transformation of CO 2 into high value-added product is a promising pathway for utilizing CO 2 . However, the process tends to require harsh reaction conditions owing to CO 2 chemical inertness. Designing a high efficiency catalytic system with environmentally benign characteristic are important determinants. In this work, protic ionic liquids [TMG][2-OPy] were prepared via one-step neutralization between 1,1,3,3-tetramethylguanidine and 2-hydroxypyridine, applying to the domain of synthesizing quinzoline-2,4(1H , 3H) - diones from CO 2 and 2-aminobenzontiles without any solvent or metal, achieving the yield of 97% at 90 °C for 8 h under atmospheric. A series of substrates with good to acceptable yield were detected, revealing the generality and universality of the catalyst. Furthermore, the system could be facilely reused for at least six runs, retaining the yield of 94%. A preliminary kinetic equation is calculated with the activation energy of 68 kJ·mol −1 , and a plausible reaction mechanism was put forward. This study highlights that the [TMG][2-OPy] enables to activate CO 2 carboxylation efficiently.
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ChemistrySelect
·
2023
·Vol. 8
·期 45
·e202300253
·
IF 2.1
Deqin Zhu,Xiaoxiao Xu,Jingjing Liu,Wenbo Lan,Ligang Wei,Kunlan Li,Na Liu,Qingda An,Guolin Shao,Shangru Zhai
Graphical Preparation of CNFs with pretreatments of inexpensive alkanolamine-based PILs with dimeric oxalic acid anions was investigated. Cation type and PIL content influenced the yields and physicochemical properties of prepared CNFs. The cations and anions in PILs cooperatively enhanced CNFs production. CNF yield of 85.0 % was obtained with [MEA][(HOA)(H 2 OA)] 30% . Preparation of cellulose nanofibrils (CNFs) with the pretreatments using alkanolamine-based protic ionic liquids (PILs) with dimeric oxalic acid anions ([(HOA)(H 2 OA)] − ) was fully investigated. The cation type [ethanolamine ([MEA] + ), diethanolamine ([DEA] + ), triethanolamine ([TEA] + )], and water addition greatly influenced the CNF yields. Under the pretreatment conditions of 110 °C and 3 h, the CNF yields with different PIL-based systems followed the order: [MEA][(HOA)(H 2 OA)]>[DEA][(HOA)(H 2 OA)]>[TEA][(HOA)(H 2 OA)], similar to their swelling capacities. The highest CNF yield of 85.0 % was obtained after the pretreatment with [MEA][(HOA)(H 2 OA)]-water containing 30 wt % PILs. The optimal pH range of PILs-water was 1.10–1.15. The good recyclability indicated that these inexpensive PILs can be employed as a simple and efficient pretreatment system for preparing CNFs. The physicochemical properties of the prepared CNFs were greatly changed by varying the PILs’ pretreatment systems. The thermal stability of CNFs was intimately connected with the crystalline structures and hydrogen bonding modes.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Shuyue Wen,Hangzhi Wu,Xiaomin Zhang,Tao Wang,Weigao Xu,Youting Wu
Carbon capture, utilization, and storage (CCUS) are among the key technologies to achieve large-scale carbon emission reduction globally. Amino acid ionic liquids (AAILs) featuring biodegradability and biological activity are capable as eco-friendly absorbents for CO 2 capture. Herein, a series of novel AAILs are proposed via one-step hydrolysis of cheap lactams, which can act as messengers to facilitate aqueous solution of multi-tertiary-amines fast and pronounced absorption of CO 2 . Dynamic absorption experiments were carried out to indicate that [N 1111 ][Maba]-PMDETA-50 % showed a larger apparent absorption rate constant (0.282 min −1 ) than that of MDEA solution (0.043 min −1 ), demonstrating the activated role of AAILs. [N 1111 ][Maba]-PMDETA-50 % shows the exceptional absorption capacity of 0.162 g (1.0 bar) or 0.095 g (0.1 bar) of CO 2 per g absorbent at 313.2 K, respectively, surpassing all the reported formulated solution. The facilitated absorption mechanism is also illuminated from the NMR spectra. The regeneration heat (equal to absorption enthalpy) was calculated to be − 55.7 kJ·mol −1 from absorption isotherm of three different temperatures. The recyclability was evaluated from the vacuum regeneration (ten consecutive absorption–desorption cycles) and dynamic thermal regeneration, achieving the regeneration efficiency of more than 95 % and 99 %, respectively. All these experimental data indicate that the AAIL-based multi-tertiary-amines aqueous solution may be good candidate absorbent in terms of rapid efficient capture of CO 2 .
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SURFACE & COATINGS TECHNOLOGY
·
2023
·
IF 5.4
Chuping Chen,You Zhang,Shuqi Wang,Zheng Zhang,Chen Wen,Fei Chen
The wide application of Mg Li alloys is limited by the poor corrosion resistance , which needs to be improved by surface treatment. Plasma electrolytic oxidation (PEO) method is one of the most promising methods for the formation of oxide coatings on Mg Li alloys. However, the conventional PEO technique with high energy consumption causes poor coating compactness and hampers efforts to enhance corrosion resistance . In this study, various concentrations of ionic liquids (1-butyl-3-methylimidazolium tetrafluoroborate, BmimBF 4 ) are introduced into the concentrated alkaline electrolyte to facilitate the formation of a PEO coating on the surface of LA91 magnesium‑lithium (Mg Li) alloy. The influence of BmimBF 4 on PEO coatings has been investigated. The results indicate that a concentrated electrolyte significantly lowers the working voltage of PEO, thereby enhancing energy efficiency. Uneven adsorption on the substrate surface, resulting from the low concentration of BmimBF 4 (≤20 mL/L) in the electrolyte, induces partial discharge, leading to high surface roughness and the formation of large pores. However, when an excessive amount of BmimBF 4 (>20 mL/L) is present, it uniformly adsorbed onto the substrate surface during the initial stage of PEO process, forming a corrosion inhibitor layer. This leads to a consistent discharge on the surface of substrate throughout the entire PEO process, resulting in a reduction in both surface roughness and micropore size. Among these coatings, the one prepared in an electrolyte containing 20 mL/L BmimBF 4 exhibits the highest contact angle (66.8° ± 3.8°) and the best long-term corrosion resistance (hydrogen evolution rates <0.02 mL·cm −2 ·h −1 ). These properties can be attributed to the physical and chemical adsorption of BmimBF 4 , which contains hydrophobic long alkyl chains, as well as the maximum thickness with extended discharging channels. This study offers a guiding strategy for further reducing energy consumption and enhancing the corrosion resistance of PEO coatings.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Wenjie Xiong,Mingzhen Shi,Lingling Peng,Xiaomin Zhang,Xingbang Hu,Youting Wu
CO 2 and H 2 S are considered impurities in natural gas that moderate the pace of environmental health. Developing highly efficient and cost-effective absorbents is of significance for sweetening natural gas. Herein, four superbase protic ionic liquids (SPILs) were prepared in this study. Typical physical properties (density, viscosity, and decomposition temperature) were also examined at ambient pressure. These SPILs show low viscosity values at ranging from 5.1 cP to 18.3 cP at 313.2 K. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures in the range of 298.2 K to 333.2 K. Impressively, the absolute solubility of H 2 S under 0.1 bar was found to be located at 4.31–5.15 mol/kg at 313.2 K, which is the highest value obtained among the reported results in the literature. The ideal selectivity of H 2 S/CH 4 and CO 2 /CH 4 (H 2 S or CO 2 solubility at 0.1 bar vs CH 4 solubility at 1 bar) at 313.2 K are in the ranges of 367–653 and 92.4–240, respectively. The interaction mechanism we explored was characterized by NMR and FT-IR spectroscopy. Thermodynamic parameters, such as enthalpy, Gibbs free energy, and entropy of dissolution were calculated from the temperature dependent solubility using the “deactivated model”. These SPILs are promising alternative candidates for the simultaneous removal of H 2 S and CO 2 in natural gas upgrading.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Wen-Long Xu,Jia-Yin Zhang,Ning-Ning Cheng,Zi-Liang Li,Hong-Chao Lan,Wen-Jing Jiang,Hai-Long Peng,Kuan Huang,Jun Du
Aminopolycarboxylate ILs (APC-ILs)—a kind of anion-grafted amine-functionalized ILs enabling 1:2 stoichiometry of reaction with CO 2 —were dispersed in mesoporous organic polymer to achieve a new class of adsorbents. The mesoporous organic polymer selected herein is polydivinylbenzene (PDVB) that can be facilely synthesized by a solvothermal route without any templates. The prepared APC-IL@PDVB samples were then systematically characterized and investigated for carbon capture performance. It is found that APC-IL@PDVB samples can efficiently adsorb CO 2 from dilute source, with the highest CO 2 capacity of 1.65 mmol/g and IL utilization ratio of 1.53 mol/mol at 30 ℃ for 10 vol% of CO 2 balanced in N 2 . The CO 2 capacities of APC-IL@PDVB samples surpass the values of most other solid-dispersed ILs, and the IL utilization ratios surpass the values of most non-dispersed ILs. The adsorption of CO 2 by APC-IL@PDVB samples is also highly selective towards N 2 , and reversible throughout consecutive adsorption-desorption cycles. Therefore, dispersing APC-ILs in PDVB is an effective approach to obtain adsorbents with high efficiency and improved performance for carbon capture from dilute source.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ruibing Bai,Junfeng Wang,Daoguang Wang,Yanqiang Zhang,Junjie Cui
The high acidity of stripping is one of the major problems that hinder the industrialization of the tributyl phosphate (TBP) + FeCl 3 system for lithium extraction from the salt lake brines with high Mg/Li ratio. In this study, a novel solvent extraction system, trialkylmethylammonium di(2-ethylhexyl)orthophosphinate ([N 1888 ][P 507 ]) + TBP + FeCl 3 , was developed to significantly reduce the difficulty of stripping and simplify the extraction process. The conditions of extraction and stripping were systematically studied in the present work. The results showed that Li + extraction efficiency could reach 61% under the optimal extraction parameters and Li + stripping ratio was 90% with a relative mild conditions of O/A = 10:1, [HCl] aq = 1.5 mol·L –1 . Also, combined with experimental results, FT-IR analysis, and UV analysis, the possible mechanisms of lithium extraction and stripping were put forward. Li + was extracted from the aqueous phase through the formation of [Li·2TBP][FeCl 4 ] adduct, meanwhile [N 1888 ][P 507 ] was just slightly involved in the extraction step. In the stripping procedure, the interaction between [FeCl 4 ] − and [Li·2TBP] + might be destroyed, and new possible complexes, [Li·2TBP] + , and [FeCl 4 ·TBP·P 507 ] 2− /[FeCl 4 ·P 507 ] 2− were formed in the organic phase. Additionally, the extraction efficiency of Li + remained above 70% while the organic phase was reused for six cycles. Compared with the traditional system, the addition of [N 1888 ][P 507 ] resulted in a slight decrease of Li + extraction efficiency (about 5%), the stripping acidity significantly reduced from 6 mol·L –1 HCl to 1.5 mol·L –1 HCl. This new extraction system showed a promising performance in selective extracting and easy stripping in lithium separation from the salt lake brines with high Mg/Li ratio.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yi Zhang,Yu Deng,Weidong Guo,Donghao Liu,Yigang Ding
Developing the efficient ionic liquid (IL)-based extractants for the solvent extraction of the rare earth elements (REEs) is crucial but still facing challenges. In this study, two carboxylic acid-functionalized upper critical solution temperature (UCST)-type ILs, N-carboxymethylpyridinium bis(trifluoromethylsulfonyl)imide ([HbetPy][Tf2N]) and N-carboxymethyl-N-methylmorpholinium bis(trifluoromethylsulfonyl)imide ([HbetMor][Tf2N]), are successfully synthesized and characterized. The extraction and separation performance toward scandium [denoted as Sc(III)] in nitrate medium aqueous solution have been carefully investigated in the homogeneous liquid–liquid extraction system under different conditions (e.g., equilibrium time, initial acidity, salting-out agent concentration, and REE concentration). The results reveal that the enhanced extractabilities of Sc(III) can be observed in homogeneous extraction compared to the biphasic system owing to the improved metal ion transfer and accelerated extraction kinetics. Meanwhile, [HbetPy][Tf2N] and [HbetMor][Tf2N] both illustrate high selectivity for Sc(III) separated from another five REEs (including La, Nd, Eu, Ho, and Yb), with the separation factors of 749 and 499 for Sc(III)/Yb(III), respectively. Moreover, the mechanism investigation indicates the formation of the Sc(III) complex via a proton exchange, evolved from the slope analysis and Fourier-transform infrared results. This study provides a prototype for the construction of the homogeneous liquid–liquid extraction system via the novel UCST-type ILs for highly efficient REE extraction and supplies the future application for the recovery of REEs from wastes.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Dingkun Lu,Chang Liu,Menghan Qin,Jingjing Deng,Guoyue Shi,Tianshu Zhou
Sulfonamides antibiotic residues are commonly found in environmental samples, which is highly concerning for public safety and environmental protection. The detection of sulfonamides antibiotics (SAs) is quite important but challenging. In this work, functionalized Zr metal-organic frameworks (Zr-MOFs) and imidazole-based ionic liquids (ILs) were selected and designed according to the structures and properties of SAs. By supporting functionalized ILs into the water-stable Zr-MOFs, the novel ILs@Zr-MOFs nanocomposites were synthesized for the pretreatment of SAs. [H 2 Nmim][NTf 2 ]@UiO-66-Br showed good selectivity for SAs with maximum adsorption capacity of 352.1 mg g −1 for sulfadiazine . The satisfied performance attributed to not only the large BET surface areas, but also the multiple interactions between the adsorbent and SAs, including electrostatic interaction , hydrogen bonding interaction and π-π interaction. The as-prepared nanocomposites were applied to the dispersive solid phase extraction of SAs in environmental water samples. Combined with high performance liquid chromatography-diode array detector (HPLC-DAD), the effective extraction and sensitive analysis of SAs was achieved by [H 2 Nmim][NTf 2 ]@UiO-66-Br with enrichment factors higher than 270 and extraction recoveries between 90.5% and 101.9% in short extraction time (10 min). The detection limits were lower than 0.03 μg L −1 .
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PubMed
高影响因子
RARE METALS
·
2020
·Vol. 40
·期 7
·1987-1994
·
IF 2.161
Wang Ya-Ting,Liu Men,Tang Nian,Li Sheng-Jian,Sun Yan,Wang Shi-Xiong,Yang Xiang-Jun
Abstract Solvent extraction based on ionic liquids is generally considered to be an environmentally benign and effective technology for gold(I) recovery. The aim of this work is to study gold(I) extraction from aurocyanide solution using fluorine-free ionic liquids [A336][SCN], [A336][MTBA] and [A336][Mal]. Various factors that affect gold(I) extraction (including concentration of ionic liquids, equilibrium pH, concentration of the modifier tributyl phosphate (TBP), reaction time and initial concentration of gold in an aqueous solution) were studied and optimized. The results indicate that the three Aliquat 336-based ionic liquids all exhibit excellent behaviors for gold(I) extraction. More than 99.8% of gold(I) can be extracted from the aqueous phase into the ionic liquid phase. The gold-loaded ionic liquids were characterized using infrared spectroscopy and mass spectrometry to study the extraction mechanism of gold(I). The results revealed that extraction of gold(I) into the ionic liquid phase was based on an exchange reaction between the anion Au(CN)
− 2
in aqueous solution and the anion SCN − in ionic liquid [A336][SCN]. The logarithmic relationship between distribution coefficient and TBP concentration indicates that two TBP molecules are involved in the formation of the extracted complex. The extracted complex was determined to be A336 + ·Au(CN)
− 2
·2TBP. In addition, the gold(I)-loaded ionic liquids can be efficiently stripped using NH 4 SCN, 2-methylthiobenzoic acid and methyl maltol. The results establish that Aliquat 336-based ionic liquids have potential application prospects in gold(I) recovery from cyanide solutions.
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危险品化学品经营许可证（带存储）