Choline chloride + levulinic acid deep eutectic solvent is studied as a suitable material for CO2 capturing purposes. The most relevant physicochemical properties of this solvent are reported together with the CO2 solubility as a function of temperature. The corrosivity of this solvent is studied showing better performance than amine-based solvents. A theoretical study using both density functional theory and molecular dynamics approaches is carried out to analyze the properties of this fluid from the nanoscopic viewpoint, and their relationship with the macroscopic behavior of the system and its ability for CO2 capturing. The behavior of the liquid-gas interface is also studied and its role on the CO2 absorption mechanism is analyzed. The reported combined experimental and theoretical approach leads to a complete picture of the behavior of this new sorbent with regard to CO2, which together with its low cost, and the suitable environmental and toxicological properties of this solvent, lead to a promising candidate for CO2 capturing technological applications.

A potential of natural deep eutectic solvent (NADES) produced with the mixture of choline chloride with lactic acid, malic acid, citric acid and fructose is studied in this work. Experimental techniques are used to collect thermophysical property data including water content, thermal strength, density and gas solubility of CO2 and N2 data at pressures up to 50 bars. Detailed rheological measurements and various models have been studied to describe the dynamic flow behavior. Moreover, a density functional theory (DFT) and classical molecular dynamics (MD) methods have been used for investigating the physicochemical properties, structuring, dynamics and interfacial behavior of the studied NADES from the nanoscopic point of view to infer its viability for extensive usage. The rheological experimental results show usual shear‐thinning effect in which the η is decreasing with shear rate at all temperatures. A trend of studied NADES viscosity profiles were found as very similar to that of common ionic liquids that were previously, where the viscosities of all studied NADES decreased with increasing temperature. DFT simulations yielded with an accurate quantification of short‐range interaction but liquid state is also characterized by middle and long‐range interaction together with volumetric effects. Molecular orientations were quantified by radial distribution functions and the developed interactions are topologically characterized.

Organic compounds, such as covalent organic framework, metal-organic frameworks, and covalent organic polymers have been under investigation to replace the well-known amine-based solvent sorption technology of CO2 and introduce the most efficient and economical material for CO2 capture and storage. Various organic polymers having different function groups have been under investigation both for low and high pressure CO2 capture. However, search for a promising material to overcome the issues of lower selectivity, less capturing capacity, lower mass transfer coefficient and instability in materials performance at high pressure and various temperatures is still ongoing process. Herein, we report synthesis of six covalent organic polymers (COPs) and their CO2, N2, and CH4 adsorption performances at low and high pressures up to 200 bar. All the presented COPs materials were characterized by using elemental analysis method, Fourier transform infrared spectroscopy (FTIR) and solid state nuclear magnetic resonance (NMR) spectroscopy techniques. Physical properties of the materials such as surface areas, pore volume and pore size were determined through BET analysis at 77 K. All the materials were tested for CO2, CH4, and N2 adsorption using state of the art equipment, magnetic suspension balance (MSB). Results indicated that, amide based material i.e. COP-33 has the largest pore volume of 0.2 cm(2)/g which can capture up to the maximum of 1.44 mmol/g CO2 at room temperature and at pressure of 10 bar. However, at higher pressure of 200 bar and 308 K ester-based compound, that is, COP-35 adsorb as large as 144 mmol/g, which is the largest gas capturing capacity of any COPs material obtained so far. Importantly, single gas measurement based selectivity of COP-33 was comparatively better than all other COPs materials at all condition. Nevertheless, overall performance of COP-35 rate of adsorption and heat of adsorption has indicated that this material can be considered for further exploration as efficient and cheaply available solid sorbent material for CO2 capture and separation.

Simple ionic liquids (containing one type of cation with one type of anion) and complex mixed ionic liquids (containing several types of anions and cations, double salts) based on ammonium cations were studied in this work using a combined computational and experimental approach. Theoretical studies were carried out using classical molecular dynamics simulations. The properties and structure of these fluids and their changes upon CO 2 absorption were analyzed. The fluids' structural, energetic, and dynamic properties were considered as a function of the type of ions composing the ionic liquids together with their changes when CO 2 is present as a function of CO 2 concentration. Likewise, experimental measurements analyze carbon capturing abilities for the studied mixed ionic liquids as a function of pressure and temperature. The reported results show that mixing two neat ammonium-based ionic liquids does not change remarkably the properties of the involved neat ionic liquids, and also the affinities for CO 2 are also similar in the mixed ionic liquids. Therefore, vastly different ions should be considered when mixed ionic liquids are designed for stimulating CO 2 physisorption by increasing the available volume and tuning affinity toward CO 2 . This work provides a nanoscopic and macroscopic characterization of complex ionic liquids and their ability for carbon capturing for the first time.

Montmorillonite nanoclay was studied for its capability of storing carbon dioxide, methane, and nitrogen at elevated pressures. Adsorption data were collected to study and assess the possible applications of montmorillonite to gas storage, as it is available in depleted shale reservoirs. The thermodynamic properties of montmorillonite and its amine impregnated structures were studied in this manuscript. Material characterization via Brunauer−Emmett−Teller analysis, thermogravimetric analysis, Fourier transform infrared and energy dispersive X-ray spectroscopies, and scanning electron microscopy was carried out on the nanoclay samples followed by low-and high-pressure gas sorption experimental measurements via high-pressure magnetic suspension sorption apparatus at 298 and 323 K isotherms up to 50 bar. Selectivities of each gas on each nanoclay material is calculated based on single gas adsorption measurements and presented in the manuscript. Additionally, heat of adsorption and kinetics of adsorption are calculated and reported.

Carbon dioxide solubility in four ionic liquids (ILs) of different families with different cationic−anionic groups (tributylmethylphosphonium formate, butyltrimethylammonium bis(trifluoromethyl sulfonyl) imide, 1-methyl-1-propylpyrrolidinium dicyanamide, and 1ethyl-3-methylimidazolium acetate) at temperature of 298 K and a pressure range from vacuum to 10 bar were studied in this work using state of the art gravimetric sorption experiments. This work provides insight information regarding CO 2 solubility for IL−IL mixing effect pressures up to 10 bar and at 298 K. Density values were used to calculate molar volume of ionic liquids for further discussions on CO 2 solubility-molar volume relationship. Noticeably higher CO 2 solubility with IL−IL hybridized systems of different family is opening a new window for research on a molecular level by simulations and intellectually designed ILs. Chemisorption behavior has been observed for the ILs that contain acetate-based anions in the structure and relevant discussion is included in this work.

Porous solid sorbents have been investigated for the last few decades to replace the costly amine solution and explore the most efficient and economical material for CO2capture and storage.