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Alkyl glycosides are biodegradable surfactants with excellent physico-chemical properties. Although their wide-range application is considered ecofriendly, their synthesis is not due to the need for toxic organic solvents and corrosive acids as catalysts. Moreover, chemical synthesis results in complex mixtures rather than defined compounds. To overcome both disadvantages as well as the limited solubility of sugars in organic solvents, a highly selective enzymatic synthesis was set up with a β-glucosidase condensing D-glucose and different fatty alcohols in a deep eutectic solvent.

Dispersive liquid-liquid microextraction is one of the most widely used microextraction techniques currently in the Analytical Chemistry field, mainly due to its simplicity and rapidity. The operational mode of this approach has been constantly changing since its introduction, adapting to new trends and applications. Most of these changes are related to the nature of the solvent employed for the microextraction. From the classical halogenated solvents (e.g., chloroform or dichloromethane), different alternatives have been proposed in order to obtain safer and non-pollutants microextraction applications. In this sense, low density solvents, such as alkanols, switchable hydrophobicity solvents and ionic liquids were the first and most popular replacements for halogenated solvents, which provided similar or better results than these classical dispersive liquid-liquid microextraction solvents. However, despite the good performances obtained with low density solvents and ionic liquids, researchers have continued investigating in order to obtain even greener solvents for dispersive liquid-liquid microextraction. For that reason, in this review, the evolution over the last five years of the three types of solvents already mentioned and two of the most promising solvent alternatives (i.e., deep eutectic solvents and supramolecular solvents), have been studied in detail with the purpose of discussing which one provides the greenest alternative. This article is protected by copyright. All rights reserved.

A new and efficient extraction procedure was proposed and used for the simultaneous extraction of four hydroxylated metabolites polycyclic aromatic hydrocarbons from urine samples. The extraction procedure was started by dissolving an organic polymer into a water-miscible organic solvent (iso-propanol) and its injection into the sample solution. The sorbent was re-precipitated in all parts of the solution as tiny particles and the analytes were adsorbed onto the sorbent. After that, the sorbent was separated and the adsorbed analytes were eluted by choline chloride: dichloroacetic acid deep eutectic solvent. The elution solvent was mixed with choline chloride-3,3-dimethyl butyric acid deep eutectic solvent and the mixture was applied in dispersive liquid-liquid microextraction procedure for more concentration of the analytes. After optimization, the method validation was followed according to International Council Harmonization guidelines and the results showed that wide linear ranges (26-500 000 ng/L) and low limits of detection (3.6-7.2 ng/L) and quantification (11-26 ng/L) were obtained. Satisfactory enrichment factors (435-475) and extraction recoveries (87-95%), and acceptable relative standard deviations (equal or less than 8.6%) were obtained. Finally, the introduced method was successfully applied for determination of the analytes in urine samples obtained from tobacco smokers.

A liquid-liquid extraction methodology was developed for the removal of Cr(VI) from contaminated water using a novel green hydrophobic deep eutectic solvent (DES) as an efficient sole extracting agent. The hydrophobic DES was obtained by mixing choline chloride and thymol in 1:4 molar ratio at 70°C for 10 min and was denoted as ChCl-THY(1:4). The ChCl-THY(1:4) works efficiently for removal of high (20 mg/L) and low (500 µg/L) concentration of Cr(VI) from artificially contaminated natural water with >95% extraction efficiency (E%) at optimized reaction conditions (pH 2-6, 40°C). The DES was characterized by 1 H NMR and FTIR spectroscopy, and the data suggest that interaction occurs between Cl- ion of choline chloride and H atoms of thymol molecules. Physicochemical properties such as density, melting point, moisture, and solubility were studied and discussed. Herein, no sharp melting point was observed for ChCl-THY(1:4) in DSC curve. DES was regenerated using 0.1 M NaOH as stripping agent, and 50%-60% extraction efficiency could be attained in the next cycle. A plausible mechanism of interaction between Cr(VI) species and DES was also explored with the help of FTIR spectroscopy. PRACTITIONER POINTS: A novel hydrophobic DES (ChCl-THY) is prepared by mixing choline chloride and thymol at 1:4 molar ratio. ChCl-THY(1:4) is employed for the first time as sole extracting agent to remove the Cr(VI) from contaminated aqueous solution. >95% extraction efficiency was achieved by ChCl-THY(1:4) in natural water conditions at µg/L and mg/L level of contamination. Both the component used to prepare the DES are naturally abundant; hence, DES is not toxic for biota. The element present in natural water did not show any interference with extraction of Cr(VI).

Electrochemical recovery of the cobalt in deep eutectic solvent shows its promise in recycling and recovery of valuable elements from the spent lithium-ion battery due to its high selectivity and minimal environmental impacts. This work unveiled the roles of the substrates, applied potentials and operating temperatures on the performance of cobalt electrochemical recovery in a deep eutectic choline chloride + urea solvent. The solvent contains cobalt and lithium ions extracted from lithium cobalt oxides - an essential lithium-ion battery cathode material. Our results highlight that the substrate predetermines the cobalt recovery modes via substrate-cobalt interactions, which could be predicted by the cobalt surface segregation energies and crystallographic misfits. We also show that a moderate cathode potential under -1.0 V vs. silver quasi-reference electrode at 94 °C - 104 °C is essential to ensure a selective cobalt recovery at an optimal rate. We also found that the stainless-steel mesh as an optimal substrate for cobalt recovery due to its relatively high selectivity, fast recovery rate, and easy cobalt collection and substrate regeneration. Our work provides new insights on metal recovery in deep eutectic solvents and offers a new avenue to control the metal electrodeposition modes via modulation of substrate compositions and crystal structures.

Introduction In the present study, ternary deep eutectic solvent-based ultrasound-assisted extraction was developed for the efficient extraction of plantamajoside, acteoside, quercetin and kaempferol from Plantago asiatica L. Methodology Six kinds of choline chloride-based ternary deep eutectic solvents (TDESs) were prepared as potential extraction solutions. In order to obtain optimal extraction efficiency, a series of extraction conditions were investigated by single-factor test and orthogonal test. Results The extraction efficiency of choline chloride/lactic acid/ethylene glycol (ChCl-LA-EG) was much higher than that of other TDESs. ChCl-LA-EG-11 synthesised with choline chloride, lactic acid and ethylene glycol (1:4:2) was considered to have a higher extraction efficiency. The optimal ultrasound-assisted extraction conditions were as follows: water content in ChCl-LA-EG-11, 50%; extraction temperature, 70°C; ratio of solid/liquid, 20 mg/mL; ultrasonic power, 60 W; extraction time, 35 min; pH of the solution, 8. Under the optimal extraction conditions, the extraction efficiencies of plantamajoside, acteoside, quercetin and kaempferol were 3.83 ± 0.41, 4.23 ± 0.45, 0.56 ± 0.15 and 0.19 ± 0.08 mg/g, respectively. The extraction efficiency of the total target components was 9.21 ± 0.63 mg/g, which was much higher than that of conventional solvents (water, methanol, ethanol, 50% methanol, 50% ethanol). The target components were isolated efficiently from the TDES solution by an AB-8 macroporous resin column with a recovery rate of 95.6%. Conclusion This study demonstrated that TDESs possessed excellent physical and chemical properties and had enormous potential for active component extraction of traditional Chinese medicinal materials.

In the present fundamental study, selectivity and efficiency of electromembrane extraction of 50 polar basic substances (-6.7

Multifunctional or structural electrolytes are characterized by ionic conductivity high enough to be used in the electrochemical devices and mechanical performance suitable for the structural applications. Preliminary insights are provided into the combustion behavior of structural bi‐continuous electrolytes based on bisphenol A diglycidyl ether (DGEBA), synthesized using the techniques of reaction induced phase separation and emulsion templating. The effect of the composition of the structural electrolytes and external heat flux on the behavior of the formulations were studied using a cone calorimeter with gases formed during testing analyzed using FTIR. The composition of the formulations investigated was changed by varying the type and amount of the ion conductive part of the bi‐continuous electrolyte. Two ionic liquids, 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)imide (EMIM‐TFSI) and 1‐butyl‐3‐methylimidazolium tetrafluoroborate (BMIM‐BF4), as well as a deep eutectic solvent (DES) based on ethylene glycol and choline chloride, were used. The results obtained confirm that time to ignition, heat release rate (HRR), total mass loss, as well as the composition of the gases released during tests depend on the composition of the formulations. Addition of liquid electrolyte is found to reduce the time to ignition by up to 10% and the burning time by between 28% and 60% with the added benefit of reducing the HRR by at least 34%. Gaseous products such as CO2, CO, H2O, CH4, C2H2, N2O, NO, and HCN were detected for all formulations with the gases SO2, NH3, HCl, C2H4, and NH3 found to be for certain formulations only.

We optimized ultrasound-assisted alcohol-based deep eutectic solvent dispersive liquid-phase microextraction for separation and preconcentration of quercetin in wine and food samples by experimental design based on central composite design. Five different alcohol-based deep eutectic solvents were prepared and tested for quercetin extraction. The effect of important parameters and matrix components were optimized. After optimization, the determination of quercetin was performed at 385 nm using spectrophotometry. Analytical data such as detection limit, working range and preconcentration factor were found as 6.1 μg/L, 20-850 μg/L, and 120, respectively. The selectivity of the optimized extraction conditions for quercetin was investigated in the presence of different matrices. The validation of the method was investigated by reproducibility, repeatability and recovery studies, as well as by comparing the analytical results obtained from real samples with the reference method. Lastly, the recommended procedure was successfully applied for the extraction and quantification of quercetin in wine and food samples.

Compared with conventional aqueous and ionic liquid electrolytes, deep eutectic solvent (DES) are considered as electrolyte for redox flow batteries because they have a wider electrochemical window and relatively low price. In this study, CeIV /CeIII and ZnII /Zn redox couples are used as the positive and negative active materials, respectively, in an electrolyte consisting of choline chloride ethylene glycol (ethaline). The structure of CeIII in the positive electrolyte is inferred through spectrum detection. CeIV /CeIII and ZnII /Zn redox couples show a stable potential difference of 2.2 V (vs. Ag) through cyclic voltammetry. The charge and discharge performance of battery was tested at different current densities. In addition, battery performance was evaluated at different temperatures and concentrations of cerium in the electrolyte. Consequently, at a current density of 0.5 mA cm-2 at room temperature and using 1.0 m CeIII , the battery performance reaches the best coulombic efficiency of 84 %.

A three-phase homogenous liquid-liquid extraction method followed by deep eutectic solvent-based dispersive liquid-liquid microextraction has been used for the extraction and preconcentration of some phytosterols from cow milk and cream samples. In this method, cow milk or melted cream was transferred into a glass test tube and a mixture of sodium hydroxide solution (as fatty acids saponification agent) and acetonitrile (as extraction/dispersive solvent) was added to the solution. The mixture was shaken manually and placed in a water bath. After dissolving sodium chloride and centrifugation, the obtained supernatant phase (acetonitrile) was removed and mixed with ethyl methyl ammonium chloride: phenyl acetic acid deep eutectic solvent at microliter level. Under optimum conditions, low limits of detection (1.6-4.1 μg/L) and quantification (5.3-13.1 μg/L), high enrichment factors (138-207), and extraction recoveries (55-83%), and good precision (relative standard deviations ≤ 6.8%) can be obtained. The method was done on different milk and cream samples and the results showed that total phytosterols level in all samples were in the permitted level established by the National Standard Organization Guidelines, except for three cream samples.

A new extraction procedure based on combination of a solvent extraction and deep eutectic solvent based dispersive liquid-liquid microextraction has been introduced for the extraction of aflatoxin M1 from cheese samples. In this method, acetonitrile, deionized water, and n-hexane are added onto the sample and vortexed. Owning to different affinities of the substances in cheese toward the mentioned solvents, an efficient and selective extraction of the analyte is done in the acetonitrile phase. After centrifugation, the acetonitrile phase is removed and mixed with a new hydrophobic deep eutectic solvent prepared from N,N-diethanol ammonium chloride and carvacrol as an extraction solvent. The mixture is injected into deionized water, and a cloudy solution is obtained. Eventually, an aliquot of the organic phase is injected into high-performance liquid chromatography-fluorescence detection. After optimizing the effective parameters with the response surface methodology and a quadratic model, limits of detection and quantification were 0.74 and 2.56 ng/kg, respectively. The obtained extraction recovery and enrichment factor were 94% and 94, respectively. Also, intra- (n = 6) and interday (n = 4) precisions were less than or equal to 8.6% at a concentration of 5 ng/kg. The suggested method was applied to determine aflatoxin M1 in different cheese samples.

Dispersive liquid-liquid microextraction has caused more and more attention in sample preparation due to its rapid and efficient extraction process. In this study, a new terpineol-based hydrophobic deep eutectic solvent was firstly synthesized by mixing α-terpineol with 1-octanoic acid, and then applied to analysis of phenols from water samples by dispersive liquid-liquid microextraction combined with HPLC-diode array detector. Infrared spectroscopy indicated that hydrogen bonding was responsible for the formation of deep eutectic solvent between α-terpineol and 1-octanoic acid. After optimization of several parameters, such as the type and volume of deep eutectic solvent and the disperser, pH and ionic strength of sample solution, the developed method exhibited excellent extraction performance to the phenols with the enrichment factors from 27 to 32. Good linearity was acquired ranging from 5 to 5000 μg/L, and detection of limits of the proposed method for the phenols ranged from 0.15 to 0.38 μg/L. The recoveries measured by spiked samples at three concentration levels ranged from 81.6% to 99.3%, and precision was found with intra-day and inter-day relative standard deviations less than 8.7% and 9.2%, respectively. Finally, the proposed method was successfully applied to the determination of the phenols in environmental water samples. This article is protected by copyright. All rights reserved.

Instead of using organic solvents, a deep eutectic solvent (DES) composed of tetrabutylammonium bromide and imidazole (Bu4 NBr/Im) was employed as a solvent for the first time to synthesize covalent organic frameworks (COFs). Due to the low vapor pressure of the Bu4 NBr/Im-based DES, a new carboxyl-functionalized COF (TpPa-COOH) was synthesized under environmental pressure. The as-synthesized TpPa-COOH has open channels, and the DES can be removed completely from the pores. The dye adsorption performance of TpPa-COOH was examined for three organic dyes with similar molecular sizes: one anionic dye (eosin B, EB) and two cationic dyes (methylene blue, MB and safranine T, ST). TpPa-COOH showed an excellent selective adsorption effect on MB and ST. The electronegative keto form in TpPa-COOH might help to form electrostatic and π-π interactions between the π-stacking frameworks of TpPa-COOH and the positive plane MB and ST molecules. The adsorption isotherms of MB and ST on TpPa-COOH were further investigated in detail, and the equilibrium adsorption was well modeled by using a Langmuir isotherm model. Together with hydrogen bonding, TpPa-COOH showed higher adsorption capacity for ST than for MB (1135 vs. 410 mg g-1 ). These results could provide a guidance for the green synthesis of adsorbents in removing organic dyes from wastewater.

A solid-phase extraction method combined with deep eutectic solvent-based dispersive liquid-liquid microextraction has been developed for the extraction of three antibiotics in honey samples prior to their determination by ion mobility spectrometry. In this method, first, a multiwall carbon nanotube/urea-formaldehyde nanocomposite was synthesized using co-precipitation polymerization method and then it was used as a sorbent for the analytes extraction from the samples. After that the adsorbed analytes were eluted from the sorbent using a water-miscible organic solvent. The collected elution solvent was mixed with tetrabutylammonium chloride:butanol deep eutectic solvent and the mixture was applied in the following microextraction method. The method provided low limits of detection and quantification in the ranges of 0.32-0.86 and 1.1-2.9 ng/g, respectively. The method had a proper repeatability expressed as relative standard deviation less than or equal to 9.1%. The validated method was successfully performed on different honey samples obtained from different producers.

BACKGROUND: Deep eutectic solvents (DESs) have been tested as promising green solvents for the microwave‐assisted extraction of phenolic compounds from brewer's spent grain (BSG). Firstly, a preliminary screening with four different DESs was carried out in order to determine the most effective DES for recovering phenolic compounds (measured as total phenols) from BSG. Later, an experimental design using the DES found to be most effective in the preliminary screening was applied to optimize microwave‐assisted choline chloride (ChCl):glycerol extraction. RESULTS: ChCl:glycerol was the most effective DES tested in the preliminary screening to recover phenolic compounds (2.3 mg GA g⁻¹ BSG), even more than methanol (80% v/v) as conventional solvent (1.2 mg GA g⁻¹ BSG). On the other hand, using ChCl:glycerol as DES, a total phenols content of 2.89 mg GA g⁻¹ BSG was obtained operating at 100 °C for 13.30 min and 37.46% (v/v) water in the DES, ferulic and coumaric acids being the most abundant. Moreover, a residual extracted solid with non‐disturbed structural carbohydrates was achieved, which could be successfully used in a biorefinery to obtain other products, such as biofuels or chemicals. CONCLUSIONS: The suitability of a novel and green extraction process based on DESs combined with microwave assistance for the recovery of phenolic compounds from BSG was demonstrated. © 2020 Society of Chemical Industry (SCI)

It is possible to prepare elastic and thermoreversible gel electrolytes with significant electroactivity by dissolving minimal weight fractions of ultra-high molecular weight polyethylene oxide (UHMW PEO) in an aluminum deep eutectic solvent (DES) electrolyte composed of AlCl and urea at a molar ratio of 1.5 : 1 (AlCl/urea). The experimental vibrational spectra (FTIR and Raman) provide valuable information on the structure and composition of the gel electrolyte. However, the complexity of this system requires computational simulations to help interpretation of the experimental results. This combined approach allows us to elucidate the speciation of the DES liquid electrolyte in the gel and how it interacts with the polymer chains to give rise to an elastic network that retains the electroactivity of the liquid electrolyte to a very great extent. The observed reactions occur between the ether in the polymer and both the amine groups in urea and the aluminum species. Thus, similar elastomeric gels may likely be prepared with other aluminum liquid electrolytes, making this procedure an effective way to produce families of gel aluminum electrolytes with tunable rheology and electroactivity., This work was financed by SALBAGE project funded by the European Union under the H2020-FETOPEN-1-2016-2017 call (GA n° 766581). The authors are very grateful to Dr. Gary Ellis for making the recording of the Raman spectra possible, and to the researchers in the SALBAGE consortium, especially Dr. Ana López- Cudero for fruitful discussions

The penetration mechanism of choline chloride‐glycerol deep eutectic solvent (DES) through the stratum corneum (SC) as a potential solvent for a novel enhancer of protein penetration into the skin was investigated in a wide and small angle X‐ray diffraction study. We found that DES penetrated through intercellular lipids but not the corneocytes. DES seemed to extract a portion of lipids of the short lamellae in the SC. Hydrated DES with a DES to water weight ratio of 9 to 1 (9DES‐1H2O) showed the strongest interaction with the lipids in the SC compared with water, DES, and hydrated DESs with another weight ratio of DES to water (DES : water=8 : 2). In a skin penetration test with a fluorescently labelled lysozyme, 9DES‐1H2O increased the amount of penetration through the SC by two‐fold compared with HEPES buffer., Drug delivery: The penetration mechanism of choline chloride‐glycerol deep eutectic solvent (DES) through the stratum corneum (SC) as a potential solvent for a novel enhancer of protein penetration into the skin was investigated in an X‐ray diffraction study. We found that hydrated DES increased the penetration of lysozyme through the SC due to the disruption of the short lipid lamellar structures through partial extraction of lipids in the SC.

Oxidative anion insertion into graphite in an aqueous environment represents a significant challenge in the construction of aqueous dual-ion batteries. In dilute aqueous electrolytes, the oxygen evolution reaction (OER) dominates the anodic current before anions can be inserted into the graphite gallery. Herein, we report that the reversible insertion of Mg-Cl superhalides in graphite delivers a record-high reversible capacity of 150 mAh g-1 from an aqueous deep eutectic solvent comprising magnesium chloride and choline chloride. The insertion of Mg-Cl superhalides in graphite does not form staged graphite intercalation compounds; instead, the insertion of Mg-Cl superhalides makes the graphite partially turbostratic.

Deep eutectic solvents have received increasing attention over the past decade, and the green and versatile nature makes them important media for developing environmentally friendly and sustainable technologies. In addition to act as green alternatives to traditional organic solvents, deep eutectic solvents offer tremendous opportunities to produce different kinds of emerging functional materials. The present review highlights the recent development and applications of deep functional materials based on deep eutectic solvents as novel adsorbents for diverse analytes in complex matrices. The type, preparation, and unique properties of deep eutectic solvents, the synthesis of deep eutectic solvent derived materials, as well as their applications in chromatographic separation are described. We aim to demonstrate that deep eutectic solvents not only allow the design of eco-friendly extraction processes but also open straightforward access to advanced materials in sample preparation.

A lactic acid/chlorine chloride-based deep eutectic solvent (DES) was used for the extraction of high-purity lignin (up to 94.7 %) in high yield (up to 75 %) from the hydrolysis/fermentation residue corn stover hydrolysate (CSH), which was generated from a pilot-plant-scale biorefinery. A range of extraction conditions were investigated, which involved varying reaction temperature, time, and DES composition. The relationship between lignin yield, purity, and structural characteristics with DES treatment conditions was determined. The extraction of high-purity lignin from hydrolysis/fermentation residues presents a promising approach for enhancing the economic feasibility of a lignocellulose biorefinery. It was also determined that DES extraction can produce lignin with a controlled range of molecular weight and functional group content.

In this work, a novel quick, easy, cheap, effective, rugged, and safe technique with hydrophobic natural deep eutectic solvent as both extractant and analyte protectant was developed and combined with gas chromatography-tandem mass spectrometry to analyze pyrethroid residues in tomatoes. Eight hydrophobic natural deep eutectic solvents were first evaluated as analyte protectants and those with decanoic acid or lactic acid as hydrogen bond donor were demonstrated to be effective in compensating for the matrix effects of pyrethroids in the gas chromatography system. Hence, they were added to solvent standards for correcting the quantitation errors instead of matrix-matched calibration standards. Then the abilities of these acid-based deep eutectic solvents to extract pyrethriods from tomatoes were evaluated. Results showed the recoveries of all pyrethroids reached to over 80% with only 5 mL menthol:decanoic acid (1:1) used, and good phase separation was easily achieved without the addition of inorganic salt in the extraction step, indicating hydrophobic natural deep eutectic solvent could be a green substitute for acetonitrile in the quick, easy, cheap, effective, rugged, and safe extraction. Compared with the conventional method, the proposed protocol improved the recoveries, reduced the matrix effects, and simplified the extraction step, demonstrating to be an effective, fast, and green method.

A green extractant, hydrophobic deep eutectic solvent was first introduced for extraction of tetracycline, oxytetracycline, and chlortetracycline from environmental water samples prior to high-performance liquid chromatography determination. Deep eutectic solvents consist of methyltrioctylammonium chloride and various medium-chain alcohols/acids, and are easy in preparation, low cost and toxicity, desirably biodegradable, and biocompatible. The overall time required for sample preparation was 6 min and the volume of organic solvent used for extraction was only 400 µL. Under the optimized extraction condition, the present method yielded low limit of detection (0.5-2.0 ng/mL), acceptable precision (relative standard deviations < 9.7%), good linearity from 2.0 to 500 ng/mL (r2 ≥ 0.9991). This optimized procedure was applied for determination of tetracyclines in different water samples with desirable spiked recovery ranged from 77.5 to 87.6%. There is, therefore, a great potential to further expand application of the method for investigation of other ultra-trace analyte(s) in environmental matrixes.

In situ synthesis of a deep eutectic solvent and homogeneous liquid-liquid microextraction performed in a narrow bore tube was developed for efficient extraction of irgaphos 168 and irganox 1010 in doogh and water samples packed in polypropylene packages. First, pH of the aqueous sample solutions containing the analytes is adjusted at 9. Then a hydrogen bond acceptor (choline chloride) and a hydrogen bond donor (oleic acid) are dissolved in the solution and vortexed to obtain a homogeneous solution. The solution is filled into a narrow bore tube, in which its bottom was clogged by a septum. Then hydrochloric acid solution is injected into the solution by a syringe. The tube is placed in an ultrasonic bath. During this step, the droplets of choline chloride:oleic acid deep eutectic solvent are produced. The method indicated high enrichment factor (435 for irgaphos 168 and 488 for irganox 1010), low limits of detection (0.03 and 0.09 ng/mL for irgaphos 168 and irganox 1010, respectively) and quantification (0.13 and 0.29 ng/mL for irgaphos 168 and irganox 1010), good recovery (74 and 83% for irgaphos 168 and irganox 1010, respectively), and satisfactory repeatabilities (relative standard deviations ≤12%) can be obtained using the developed method.

Application of new strategies for supramolecular self-assembly can significantly impact the properties and/or functions of supramolecular polymers. To realize a facial strategy for the development of solvent-free supramolecular polymers in bulk, "deep eutectic solvents" were employed. Cyclodextrins and natural acids were used to prepare deep eutectic supramolecular polymers (DESPs). Deep eutectic solvents have special characteristics that endow DESPs with unique macroscopic properties and excellent processability. DESPs exhibit supramolecular adhesion and temperature-dependent behavior originating from the combined effects of deep eutectic solvents and supramolecular polymerization. Because DESPs are solvent-free and display interesting macroscopic properties, they have potential as new adaptive materials.