Soft Matter
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2022
·Vol. 18
·期 16
·3241-3248
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IF 4.046
Ying Zhang,Hejie Wang,Qintang Li,Xiao Chen
As novel solvents, deep eutectic solvents (DESs) are non-toxic, easily producible and biocompatible, which is attractive for eutectogel fabrication. In this work, a benzene 1,3,5-tricarboxamide (BTA) derivative (substituted by three hexanoic acid) was selected to prepare a supramolecular gel in a suitable DES composed of choline chloride and phenylacetic acid molecules. The obtained eutectogel exhibited higher stability than that produced in conventional solvents. The gel microstructure was composed of spiral fiber networks as confirmed from atomic force microscopy and scanning electron microscopy observations. Macroscopic chirality was therefore recognized by the circular dichromatic spectrum, though such a supramolecular chiral signal was random. To explore the gelation mechanism, the effect of BTA derivative molecular structure change was systematically investigated. With the help of Fourier transform infrared spectroscopy and powder X-ray diffraction, the gel formation was attributed to the π–π stacking of adjacent BTA molecules and the three-fold hydrogen bond between amide groups or the hydrogen bond between carboxylic groups. Furthermore, the directional hydrogen bonds between BTA and solvent molecules induced their aggregate to form one-dimensional fibers, which were either left- or right-handed. The obtained results not only extend the gel systems in DESs, but also help design the supramolecular chirality from non-chiral molecules.
研究领域:
材料科学
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超分子化学
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物理化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xudong Zhang,Junyao Wang,Jun Shen,Yugao Wang,Gang Liu,Yanxia Niu,Qingtao Sheng
Indole is an important organic synthesis intermediate derived from the wash oil fraction in coal tar. Deep eutectic solvents (DESs) have been widely used in the separation field due to their unique properties such as easy preparation, low cost, green and high extraction efficiency, and reusability. In this study, five DESs, including tetramethylammonium chloride/ethylene glycol (TMAC/EG), triethylmethylammonium chloride/ethylene glycol (TEMAC/EG), tetraethylammonium chloride/ ethylene glycol (TEAC/EG), tetrapropylammonium chloride/ethylene glycol (TPAC/EG), tetrabutylammonium chloride /ethylene glycol (TBAC/EG) were prepared and used to extract indole from model wash oil. The results showed that TPAC/EG exhibited the best extraction ability under the same conditions. Then, the main experimental parameters such as mass ratio of DES to model wash oil, extraction temperature, extraction time, standing time and initial concentration of indole, were investigated when using TPAC/EG as extractant. In optimal conditions (25℃, 5 min, mass ratio 1:8), the extraction efficiency, selectivity and distribution coefficient for indole were 90.51%, 79.21% and 61.12, respectively. Moreover, removing neutral oil with petroleum ether, the purity of indole further reached 96.63%, which was much higher than that in the previous studies reported. In addition, accessible and environmentally friendly water instead of diethyl ether was used to regenerate the DES. Reused four times, the TPAC/EG extraction ability for indole almost did not change. Finally, the mechanism of extraction process was investigated by FT-IR analysis. This work provides a new route for extraction and recovery indole from wash oil.
研究领域:
化学工程
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环境科学
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有机化学
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产品关联
DOI
高影响因子
Frontiers in Nutrition
·
2024
·
IF 4
Wang Zilin,Tian Yang,Yang Min,Yang Junyan,Wang Yifan,Tao Liang,Sheng Jun,Shi Chongying
Background: In this study, deep eutectic solvents (DESs) combined with ultrasound-assisted extraction (UAE) were used to extract bioactive compounds from the leaves of Moringa oleifera Lam.Methods: The FT-IR method was used to analyze the structural characteristics of the DESs, and the extraction efficiencies of the DESs for total phenolic content (TPC) and total flavonoid content (TFC) were evaluated. The stability of the extracts under high temperature and UV radiation was assessed, and their antioxidant activity was investigated after undergoing in vitro simulated digestion.Results: The results show that the seven DESs extracted more TPC and TFC than did the 70% ethanol (36.27 ± 1.58 mg GAE/g, 23.09 ± 1.47 mg RT/g), and the extraction process of UAE-DES was optimized by selecting choline chloride: citric acid as the DES solvent, which has the highest extraction of TPC (86.92 ± 1.34 mg GAE/g) and TFC (49.73 ± 0.85 mg RT/g). The stability results indicated that the DES phenolic extracts were less stable when exposed to high temperature and UV radiation, indicating that DES extracts have better bioactivity. Moreover, after in vitro simulated digestion, the DES extract shows a higher DPPH free radical scavenging capacity (12.79 ± 3.88 mmol Trolox/g of DES extracts, 6.99 ± 4.02 mmol Trolox/g of ethanol extracts) and ferric ion reducing antioxidant power (62.61 ± 1.71 mmol Trolox/g of DES extracts, 55.07 ± 1.66 mmol Trolox/g of ethanol extracts) than ethanol extracts.Conclusion: This study confirmed that DESs are a new and environmentally friendly solvent that can be used for the extraction of phenolic compounds.
研究领域:
植物化学
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食品科学
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分析化学
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生物技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2022
·Vol. 103
·期 6
·3006-3016
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IF 4.125
Xiaoxiang Han,Jianghui Huang,Jinwang Cai,Chen Yu,Shengchou Jiang,Qing Ye,Shuifen Yang,Weichun Pan,Qiaozhi Zhang,Yanbo Wang
Background As potent antioxidants, anthocyanins can protect the body from free radicals. However, the traditional solvent extraction method has the disadvantages of requiring a high extraction temperature and long extraction time, so it is necessary to develop an efficient extraction method for anthocyanins. Results In this study, the technique of natural deep eutectic solvents (DESs) was applied to extract anthocyanins from purple perilla leaves with the aid of microwave-ultrasonic assisted extraction (MUAE). The response surface methodology (RSM), based on the Box–Behnken design (BBD), predicted the maximum extraction yield of anthocyanins to be 619.62 mg (100 g) −1 under the following conditions: x 1 (ultrasonic extraction power) = 357.25 W, x 2 (time) = 25.62 min, and x 3 (temperature) = 57.80 °C. The biological activity of the extract obtained was evaluated by examining its radical-scavenging effect on 1,1-diphenyl-2-picrylhydrazyl, hydroxyl radical, and superoxide anion radicals. Its bacteriostatic impact was investigated on four typical bacteria: Shewanella putrefaciens ( S. putrefaciens ), Pseudomonas fluorescens ( P. fluorescens ), Escherichia coli ( E. coli ), and Staphylococcus aureus ( S. aureus ). Conclusion The integrated extraction method of DESs with MUAE was efficient, energy-saving, green, and sustainable. © 2022 Society of Chemical Industry.
研究领域:
食品科学
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化学工程
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植物化学
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生物技术
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Jianhua Song,Lin Xu,Xiaoping Wang,Chonghao Chen,Weichong Wang,Haoyu Long,Muhammad Asif Nawaz,Dianhua Liu
In classical homogeneous catalysis with noble metals as catalysts, catalyst separation is a major obstacle of its widespread application. It has by far still a challenge to establish a highly effective and easy-to-separate system in a rational manner. Herein, rationally tailored acidic deep eutectic solvents (ADESs) were applied as acid promoter, phase separator, and extractant in Pd-catalyzed methoxycarbonylation of ethylene, resulting in high catalytic activity and selectivity as well as long-term stability towards the desired methyl propionate (MP), along with the homogeneous catalysis and heterogeneous separation. This work represents an elegant and advanced methodology in the area of catalyst recycling, the deeper insights put forward in text are meaningful for further exploration of abundant industrial applications and deep eutectic solvents (DESs) design.
研究领域:
化学工程
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催化
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Wentao Zheng,Jialing Chen,Yujiao Jia,Nengqi Sun,Shiping Wang,Xianku Wu,Xuehua Zhang
A series of 1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU)/N-heterocyclic DESs aqueous solutions were designed and synthesized as CO 2 capture agents. They showed excellent performance in absorption capacity, especially for the low-pressure CO 2 . The CO 2 loads in the absorbents were higher than 1.0 mol/mol when the pressure was just 0.1 bar. Through a combination of 13 C NMR spectra, FT-IR spectra and absorption experiments, a novel absorption mechanism was proposed. It was the shuttling role of the carbamate generated from CO 2 and nitrogen heterocycles, along with the synergistic roles of the DBU and water, that caused the high absorption capacity of the DBU/N-heterocyclic DESs for CO 2 . Meanwhile, the thermodynamic parameters, the activation energy and the regeneration efficiency were all measured to estimate the absorption performance of the DBU/N-heterocyclic DESs aqueous solutions for low-concentration CO 2 .
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 14
·4473-4482
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IF 9.48
Shubin Wang,Zuotai Zhang,Zhouguang Lu,Zhenghe Xu
Deep eutectic solvents (DESs), as a green alternative technology, exhibit great potential to recycle valuable elements from spent lithium-ion batteries (LIBs). However, due to the weak reducing power of DESs, raising the temperature and extending the duration of processing are not efficient for screening suitable DESs for the recycling of LIBs. Here, we propose a novel, simple and robust experimental method to identify suitable DESs for recycling spent LIBs. Based on electrochemical principles, the method proposed in this study can be used to quickly determine the reducing power of DESs. As an example, a choline chloride (ChCl) and urea mixture as a DES was found to possess strong reducing power, with a Li and Co extraction efficiency of 95% from spent LIBs obtained at a reduced reaction temperature of 180 °C and reaction time of 12 h. The results are in good agreement with the results from Fukui functions calculations. The kinetic experiments revealed that the Li and Co extraction is controlled by solution and electron diffusion through the DES. Furthermore, a cubic cobalt oxide spinel (Co3O4) was obtained from the loaded DES using H2C2O4 and NaOH in the dilution–precipitation–calcination process. The current strategy demonstrates great potential for rapid and reliable screening of suitable DESs for the effective recycling of spent LIBs.
研究领域:
材料科学
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环境工程
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化学工程
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电池技术
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产品关联
DOI
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2020
·
IF 3.333
Xingquan Xiong,Hui Zhang,Shi Lin Lai,Jinbin Gao,Lizhu Gao
Lignin is a biodegradable, abundant and renewable natural polymer on earth. In this study, deep eutectic solvents (DESs)-modified lignin heterogeneous catalysts were prepared for the first time via a facile acid-base interaction between choline chloride (ChCl) and p -aminobenzoic acid (PABA) or its derivatives, which were used to efficiently catalyze the cycloaddition of CO 2 and terminal epoxides under green and mild conditions. Among them, lignin-ChCl-PABA was found to exhibit the highest catalytic activity for the cycloaddition of epoxides in the presence of 1.0 MPa of CO 2 while retaining high selectivity, which far outperformed those achieved on the homogeneous EDSs catalytic system. A series of cyclic carbonates could be obtained in high yields (90–99%), and lignin-ChCl-PABA was stable and reusable for the cycloaddition reaction (84% yield after 5 recycles). The attaching DES of ChCl/PABA onto the functional lignin increased the catalytic activity and also made the catalyst easier to recycle from the reaction mixture. The OH and NH 2 groups on the surface of lignin-ChCl-PABA played a very important role in the acceleration of the cycloaddition reaction under solvent free conditions.
研究领域:
化学工程
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材料科学
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环境化学
·
绿色化学
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催化
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Pengjiang Liu,Zihao Yang,Weidong Li,Renjie Huang,Lin Luo,Zheng Li,Miao Zuo,Lu Lin,Xianhai Zeng
The compound 5-(Chloromethyl) furfural (CMF) is a novel and versatile biobased platform molecule, possessing numerous exceptional properties that position it as an outstanding alternative to 5-Hydroxymethylfurfural (HMF). In this work, we demonstrate a green and efficient route for direct production of CMF from biomass waste corncob residue with high substrate concentration in deep eutectic solvents (DESs). Ideal CMF yields of 27.51, 21.75, 17.84, and 16.01 % could be obtained from biomass substrate concentrations of 5, 10, 15, and 20 %, respectively. The DES/Methyl isobutyl ketone (MIBK) biphasic reaction system with effective cycling performance was raised to deal with various biomass feedstocks. Subsequently, we also synthesized solid acid catalysts 0.2Al/MCM-41 and applied them to the CMF preparation, which has significant advantages in cycling performance, although their catalytic performance is relatively low. Besides, further investigation of the formation process of CMF in DES is conducted through experiments and theoretical calculations.
研究领域:
化学工程
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绿色化学
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生物质转化
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催化
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Chenxi Lu,Bingqing Hu,Liangzhi Li,Xin Ju,Lishi Yan
5-hydroxymethylfurfural (5-HMF) is a key platform chemical that can be applied to generate varied value-added products. Herein, the sulfonated zirconium/tin Mixed-Metal metal–organic frameworks (MOFs), Sn/UiO-66-SO 3 H catalysts were employed for catalytic conversion of biomass-derived carbohydrates (glucose, sucrose, maltose, starch, and cellulose) to 5-HMF in green deep eutectic solvents (DESs)-water based biphasic system. The Sn/UiO-66-SO 3 H catalysts were prepared by infiltrating Sn 4+ into the UiO-66-SO 3 H via post-synthesis modification. The synthesized catalysts were characterized by PXRD, SEM, FTIR, N 2 adsorption–desorption analysis, XPS, ICP-OES, NH 3 -TPD and Py-FTIR. The synergistic effect of Zr 4+ and Sn 4+ increased the total acidity and pore size of MOFs, thus promoting the catalytic performance of MOFs towards carbohydrates conversion to 5-HMF. The 24-Sn/UiO-66-SO 3 H with impregnation of Sn 4+ for 24 h presented desired catalytic ability, which resulted in 81.5 % and 41.7 % 5-HMF yields from glucose and cellulose in DES betaine-malic acid–water/MIBK biphasic system, respectively. Moreover, the five-recycling test for 24-Sn/UiO-66-SO 3 H demonstrated excellent reusability of the prepared catalyst. This study offered a novel sulfonated Mixed-Metal strategy on MOFs in DES betaine-malic acid–water based biphasic system for the production of 5-HMF from biomass-derived carbohydrates.
研究领域:
催化
·
绿色化学
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材料科学
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生物质转化
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化工工程
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Yuling Zhang,Hongwei Ren,Hasmerya Maarof,Syarah Mat Udin,Yize Liu,Meiyu Li,Hajar Alias,Erhong Duan
Highly efficient, reversible and green dissolution of lignin is still a challenge, which hinders its wide scale-up applications. In this study, amino acid-polyol deep eutectic solvents (DESs) by employing l -arginine ( l -Arg) and l -proline ( l -Pro) as HBA and ethylene glycol (EG) and glycerol (Gly) as HBD were prepared as well as applied for dealkaline lignin (DAL) dissolution, to explore the efficient system for lignin dissolution and unveil the solubilization mechanism. The mostly used choline chloride (ChCl) based DESs were also evaluated as controlled groups. It was found that the higher value of α (hydrogen-bond donating ability) of DESs was conducive for DAL dissolution, due to the high content of β-O-4 bond in DAL. Among all the investigated DESs at water content of 2 wt%, ChCl/LA with the highest value of α (2.35) presented the best lignin dissolving ability (29.09 wt%). The effects of water content on the lignin dissolving ability of hydrated DESs were tested and discussed detailly, from a microcosmic perspective by using Fourier transform infrared spectroscopy (FTIR), 1 H nuclear magnetic resonance ( 1 H NMR), solvatochromic parameters and quantum chemistry calculations. It was remarkable to find that added water greatly improved the mass transfer and activated the reaction sites in both l -Pro and l -Arg based DESs, thus enhancing or maintaining the lignin solubilities at high water concentrations. The hydrated l -Arg/EG DESs allowed a solubility enhancement of 3.49 and 2.16 times at 70 and 90 wt% water concentration, compared to l -Arg/EG/2 wt%H 2 O at 60 °C, which was environmentally friendly and economically attractive. However, the addition of water was a negative factor for ChCl based DESs, because water preferred to interact with Cl − with strong electronegativity, resulting in stronger interaction energy between hydrogen bond donors (HBD) and Ch + . This work provided a bridge connecting the microstructure and dissolving behavior of hydrated DESs, indicating that the addition of water could make DESs more versatile and flexible, thus boosting various potential applications such as gas capture, the dissolution and delivery of medicine.
研究领域:
化学工程
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材料科学
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环境科学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Chengxin Peng,Wanghao Li,Yue Liu,Yunjie Cao,Zhihui Niu,Jian Luo,Xiaohua Sun,Jianfeng Mao,Yulin Min,T. Leo Liu,Yu Zhao,Shi Xue Dou,Zaiping Guo
Biredox deep-eutectic solvents (DESs)-based electrolytes have shown unique features in non-aqueous asymmetrical redox flow batteries (RFBs) that can potentially mitigate the crossover issue. However, strong intermolecular interactions among the electrolyte constituents in DESs bring in practical challenges such as limited mass transfer rates, slow redox kinetics, and degraded cyclability. Here, by using a novel biredox-type DES based on 4-methoxy-2,2,6,6-tetramethyl-1-piperidinyloxy (4-MeO-TEMPO) and 3,3′-dimethylazobenzene (3,3′-Azo) as a model electrolyte system, the intermolecular interaction involving in the biredox DESs is unlocked by first-principles calculations, and their influence on the electrochemical performance of biredox DESs couples is systematically investigated in comprehensive consideration of the solvents and the supporting salts. It demonstrates that employing tetrabutylammonium bis-trifluoromethane sulfonimidate-acetonitrile as the supporting electrolyte synergistically weakens the intermolecular interactions within the DESs, thereby significantly promoting the redox kinetics and electrochemical reversibility in non-aqueous symmetrical RBFs. With such an optimized electrolyte, a prototype symmetrical cell under static mode is capable of delivering a high output voltage of ∼2.15 V, a decent cyclability, and the exceptional rate capability with a current density of 25 mA cm −2 . This study provides a simple yet effective way to develop advanced RFBs with dependable electrolyte regulation.
研究领域:
电化学
·
材料科学
·
能源存储
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）