The Influence of Hydrogen Bond Donors on the CO2 Absorption Mechanism by the Bio-Phenol-Based Deep Eutectic Solvents.
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ABSTRACT:
SUBMITTER: Wang Z
PROVIDER: S-EPMC8658771 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Amine absorption (or amine scrubbing) is currently the most established method for CO2 capture; however, it has environmental shortcomings and is energy-intensive. Deep eutectic solvents (DESs) are an interesting alternative to conventional amines. Due to their biodegradability, lower toxicity and lower prices, DESs are considered to be "more benign" absorbents for CO2 capture than ionic liquids. In this work, the CO2 absorption capacity of choline-chloride/levulinic-acid-based (ChCl:LvAc) DESs was measured at different temperatures, pressures and stirring speeds using a vapour-liquid equilibrium rig. DES regeneration was performed using a heat treatment method. The DES compositions studied had ChCl:LvAc molar ratios of 1:2 and 1:3 and water contents of 0, 2.5 and 5 mol%. The experimental results showed that the CO2 absorption capacity of the ChCl:LvAc DESs is strongly affected by the operating pressure and stirring speed, moderately affected by the temperature and minimally affected by the hydrogen bond acceptor (HBA):hydrogen bond donator (HBD) molar ratio as well as water content. Thermodynamic properties for CO2 absorption were calculated from the experimental data. The regeneration of the DESs was performed at different temperatures, with the optimal regeneration temperature estimated to be 80 °C. The DESs exhibited good recyclability and moderate CO2/N2 selectivity.
| S-EPMC8465201 | biostudies-literature
Project description:In this work, 502 experimental data for CO2 solubilities and 132 for Henry's constants of CO2 in DESs were comprehensively summarized from literatures and used for further verification and development of COSMO-RS. Large systematic deviations of 62. 2, 59.6, 63.0, and 59.1% for the logarithmic CO2 solubilities in the DESs (1:2, 1:3, 1:4, 1:5), respectively, were observed for the prediction with the original COSMO-RS, while the predicted Henry's constants of CO2 in the DESs (1:1.5, 1:2, 1:3, 1:4, 1:5) at temperatures ranging of 293.15-333.15 K are more accurate than the predicted CO2 solubility with the original COSMO-RS. To improve the performance of COSMO-RS, 502 data points of CO2 solubility in the DESs (1:2, 1:3, 1:4, 1:5) were used for correcting COSMO-RS with a temperature-pressure dependent parameter, and the CO2 solubility in the DES (1:6) was predicted to further verify the performance of the corrected model. The results indicate that the corrected COSMO-RS can significantly improve the model performance with the ARDs decreasing down to 6.5, 4.8, 6.5, and 4.5% for the DESs (1:2, 1:3, 1:4, and 1:5), respectively, and the corrected COSMO-RS with the universal parameters can be used to predict the CO2 solubility in DESs with different mole ratios, for example, for the DES (1:6), the corrected COSMO-RS significantly improves the prediction with an ARD of 10.3% that is much lower than 78.2% provided by the original COSMO-RS. Additionally, the result from COSMO-RS shows that the σ-profiles can reflect the strength of molecular interactions between an HBA (or HBD) and CO2, determining the CO2 solubility, and the dominant interactions for CO2 capture in DESs are the H-bond and Van der Waals force, followed by the misfit based on the analysis of the predicted excess enthalpies.
| S-EPMC7031488 | biostudies-literature
Project description:Deep eutectic solvents (DESs) have been widely used to capture CO2 in recent years. Understanding CO2 mechanisms by DESs is crucial to the design of efficient DESs for carbon capture. In this work, we studied the CO2 absorption mechanism by DESs based on ethylene glycol (EG) and protic ionic liquid ([MEAH][Im]), formed by monoethanolamine (MEA) with imidazole (Im). The interactions between CO2 and DESs [MEAH][Im]-EG (1:3) are investigated thoroughly by applying 1H and 13 C nuclear magnetic resonance (NMR), 2-D NMR, and Fourier-transform infrared (FTIR) techniques. Surprisingly, the results indicate that CO2 not only binds to the amine group of MEA but also reacts with the deprotonated EG, yielding carbamate and carbonate species, respectively. The reaction mechanism between CO2 and DESs is proposed, which includes two pathways. One pathway is the deprotonation of the [MEAH]+ cation by the [Im]- anion, resulting in the formation of neutral molecule MEA, which then reacts with CO2 to form a carbamate species. In the other pathway, EG is deprotonated by the [Im]-, and then the deprotonated EG, HO-CH2-CH2-O-, binds with CO2 to form a carbonate species. The absorption mechanism found by this work is different from those of other DESs formed by protic ionic liquids and EG, and we believe the new insights into the interactions between CO2 and DESs will be beneficial to the design and applications of DESs for carbon capture in the future.
| S-EPMC8836646 | biostudies-literature
Project description:The bioinspired incorporation of pendant proton donors into transition metal catalysts is a promising strategy for converting environmentally deleterious CO2 to higher energy products. However, the mechanism of proton transfer in these systems is poorly understood. Herein, we present a series of cobalt complexes with varying pendant secondary and tertiary amines in the ligand framework with the aim of disentangling the roles of the first and second coordination spheres in CO2 reduction catalysis. Electrochemical and kinetic studies indicate that the rate of catalysis shows a first-order dependence on acid, CO2, and the number of pendant secondary amines, respectively. Density functional theory studies explain the experimentally observed trends and indicate that pendant secondary amines do not directly transfer protons to CO2, but instead bind acid molecules from solution. Taken together, these results suggest a mechanism in which noncooperative pendant amines facilitate a hydrogen-bonding network that enables direct proton transfer from acid to the activated CO2 substrate.
| S-EPMC5879468 | biostudies-literature
Project description:Using the basic principle of construction between a hydrogen bond acceptor (HBA) and a hydrogen bond donor (HBD), four bio-based deep eutectic solvents (DESs) were prepared in a 1:2 molar ratio of HBA:HBD. 2,3-Dihydroxypropyl-1-triethylammonium chloride ([C9H22N+O2]Cl-) was synthesized from raw glycerol and used as an HBA. Lactic acid, urea, pure glycerol, and ethylene glycol were selected as HBD. Attempts to prepare DESs, using citric acid and benzoic acid as HBDs, were unsuccessful. All these DESs were characterized using FTIR and NMR techniques. Besides, physicochemical parameters such as pH, viscosity, density, and melting point were determined. The behavior of these DES to fractionate olive pomace was studied. Lignin recovery yields spanned between 27% and 39% (w/w) of the available lignin in olive pomace. The best DES, in terms of lignin yield ([C9H22N+O2]Cl- -lactic acid), was selected to perform a scale-up lignin extraction using 40 g of olive pomace. Lignin recovery on the multigram scale was similar to the mg scale (38% w/w). Similarly, for the holocellulose-rich fractions, recovery yields were 34% and 45% for mg and multi-gram scale, respectively. Finally, this DES was used to fractionate four fruit pruning samples. These results show that our novel DESs are alternative approaches to the ionic liquid:triethylammonium hydrogen sulfate and the widely used DES: choline chloride:lactic acid (1:10 molar ratio) for biomass processing.
| S-EPMC7248933 | biostudies-literature
Project description:The refractive index (RI) is an important physiochemical property of deep eutectic solvents (DESs) for application in the optical identification of specific substances or measuring the concentration of solutes in solutions. However, the available data on the RI of DESs is limited. Here, a systematic investigation on the RI of 48 typical DESs and 30 mixtures with water was conducted under atmospheric pressure. The effect of temperature in the range 293.15-338.15 K, hydrogen-bonding donors (HBDs), and hydrogen-bonding acceptors (HBAs) on RI was investigated. Furthermore, the RI of DESs as a function of mass percentage in the range of 20-80% water was also studied. It was found that the RI of DESs and its aqueous binary mixtures decreases linearly with the increase of temperature. HBDs and HBAs had a significant influence on the RI of DESs. Among them, the RI of choline chloride (ChCl)/phenol and ChCl/o-cresol were obviously higher than those of other DESs. It was also found that the addition of water would decrease the RI of DESs, and the RI of DES content in percentage (wt %) of water binary mixtures increases linearly as a function of mass percentage of DESs for 20 DESs. However, for the other 10 DESs, there is no linear relationship between the RI and the DES content.
| S-EPMC10357551 | biostudies-literature
Project description:Deep eutectic solvents (DESs) are eutectic mixtures of salts and hydrogen bond donors with melting points low enough to be used as solvents. DESs have proved to be a good alternative to traditional organic solvents and ionic liquids (ILs) in many biocatalytic processes. Apart from the benign characteristics similar to those of ILs (e.g., low volatility, low inflammability and low melting point), DESs have their unique merits of easy preparation and low cost owing to their renewable and available raw materials. To better apply such solvents in green and sustainable chemistry, this review firstly describes some basic properties, mainly the toxicity and biodegradability of DESs. Secondly, it presents several valuable applications of DES as solvent/co-solvent in biocatalytic reactions, such as lipase-catalyzed transesterification and ester hydrolysis reactions. The roles, serving as extractive reagent for an enzymatic product and pretreatment solvent of enzymatic biomass hydrolysis, are also discussed. Further understanding how DESs affect biocatalytic reaction will facilitate the design of novel solvents and contribute to the discovery of new reactions in these solvents.
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Project description:Deep eutectic solvents (DESs) are an emerging class of modern, often "green" solvents with unique properties. Recently, a deep eutectic system based on amphiphilic surfactant N-alkyl-N,N-dimethyl-3-ammonio-1-propanesulfonate (C12 & C14 sulfobetaine) and (1S)-(+)-10-camphor-sulfonic acid in the molar ratio 1:1.5 has been reported. Nanostructuring can be expected in this DES due to the nature of the components. In this work, we have investigated the native nanostructure in the DES comprising C12-C18 alkyl chain sulfobetaines with camphor sulfonic acid and how it interacts with polar and nonpolar species, water and dodecane, respectively, using small angle neutron scattering. By using contrast variation to highlight the relative position of the solvent components and additives, we can resolve the structure of the solvent and how it changes upon interaction with water and dodecane. Scattering from the neat DES shows structures corresponding to the self-assembly of sulfobetaines; the size of the structure increases as the alkyl chain length of the sulfobetaines increases. Water and dodecane interact, respectively, with the hydrophilic and hydrophobic moieties in the DES structure, primarily the sulfobetaine, thereby swelling and solvating the entire structure. The extent of the shift of the peak position, and the swelling, depend on concentration of the additive. The solution phase organization and the interaction of polar and nonpolar species as observed here, have the potential to affect the ordering of inorganic or polymeric materials grown in such solvents, paving new avenues for templating applications.
| S-EPMC10688184 | biostudies-literature
Project description:As functional liquid media, natural deep eutectic solvent (NADES) species can dissolve natural or synthetic chemicals of low water solubility. Moreover, the special properties of NADES, such as biodegradability and biocompatibility, suggest that they are alternative candidates for concepts and applications involving some organic solvents and ionic liquids. Owing to the growing comprehension of the eutectic mechanisms and the advancing interest in the natural eutectic phenomenon, many NADES applications have been developed in the past several years. However, unlike organic solvents, the basic structural unit of NADES media primarily depends on the intermolecular interactions among their components. This makes NADES matrices readily influenced by various factors, such as water content, temperature, and component ratio and, thus, extends the metabolomic challenge of natural products (NPs). To enhance the understanding of the importance of NADES in biological systems, this review focuses on NADES properties and applications in NP research. The present thorough chronological and statistical analysis of existing report adds to the recognition of the distinctiveness of (NA)DES, involves a discussion of NADES-related observations in NP research, and reportes applications of these eutectic mixtures. The work identifies potential areas for future studies of (NA)DES by evaluating relevant applications, including their use as extraction and chromatographic media as well as their biomedical relevance. The chemical diversity of natural metabolites that generate or participate in NADES formation highlights the growing insight that biosynthetically primordial metabolites (PRIMs) are as essential to the biological function and bioactivity of unrefined natural products as the biosynthetically more highly evolutionary metabolites (HEVOs) that can be isolated from crude mixtures.
| S-EPMC5913660 | biostudies-literature
Project description:This article provides an overview of a deep eutectic mixture based on the application of lithium nitrate (V) and acetamide as an electrolyte in a carbon-based electrochemical capacitor. This type of electrolyte is intended to be applied in devices designed for operation under critical conditions (e. g., extreme temperatures). In contrast to water- and common organic-based formulations, the proposed electrolyte ensures good device performance at 100 °C. To describe the chemistry of the proposed mixture, infrared and Raman spectroscopy, differential scanning calorimetry, and gas chromatography with mass spectrometry were used. Electrochemical analysis includes the verification of system ageing, self-discharge monitoring, leakage current measuring, and fundamental testing related to determining the specific capacitance or maximum voltage. Additionally, comprehensive analysis of the lithium nitrate salt and organic solvent addition to the operating system was carried out, including the replacement of lithium ions with sodium or potassium.
| S-EPMC8596588 | biostudies-literature