scholarly journals Quantum Chemistry Insight into the Interactions Between Deep Eutectic Solvents and SO2

Molecules ◽  
2019 ◽  
Vol 24 (16) ◽  
pp. 2963 ◽  
Author(s):  
Mert Atilhan ◽  
Tausif Altamash ◽  
Santiago Aparicio
Keyword(s):  
Density Functional ◽  
Rational Design ◽  
Molecular Level ◽  
Research Work ◽  
Deep Eutectic Solvents ◽  
Systematic Research ◽  
Capture Process ◽  
Interaction Sites ◽  
So2 Capture ◽  
Reduced Density

A systematic research work on the rational design of task specific Deep Eutectic Solvents (DES) has been carried out via density functional theory (DFT) in order to increase knowledge on the key interaction parameters related to efficient SO2 capture by DES at a molecular level. A total of 11 different DES structures, for which high SO2 affinity and solubility is expected, have been selected in this work. SO2 interactions in selected DES were investigated in detail through DFT simulations and this work has generated a valuable set of information about required factors at the molecular level to provide high SO2 solubility in DES, which is crucial for enhancing the current efficiency of the SO2 capture process and replacing the current state of the art with environmentally friendly solvents and eventually implementing these materials in the chemical industry. Results that were obtained from DFT calculations were used to deduce the details of the type and the intensity of the interaction between DES and SO2 molecules at various interaction sites as well as to quantify short-range interactions by using various methods such as quantum theory of atoms in a molecule (QTAIM), electrostatic potentials (ESP) and reduced density gradients (RDG). Systematic research on the molecular interaction characterization between DES structures and SO2 molecule increases our knowledge on the rational design of task-specific DES.

scholarly journals A density functional theory insight towards the rational design of ionic liquids for SO2 capture

2015 ◽  
Vol 17 (20) ◽  
pp. 13559-13574 ◽  
Author(s):  
Gregorio García ◽  
Mert Atilhan ◽  
Santiago Aparicio
Keyword(s):  
Density Functional Theory ◽  
Ionic Liquids ◽  
Density Functional ◽  
Rational Design ◽  
Molecular Level ◽  
Gas Solubility ◽  
Functional Theory ◽  
So2 Capture

A systematic density functional theory (DFT) analysis has been carried out to obtain information at the molecular level on those factors related to efficient SO2 capture by ionic liquids. A set of 55 ionic liquids, for which high gas solubility is expected, has been selected.

scholarly journals Systems Analysis of SO2-CO2 Co-Capture from a Post-Combustion Coal-Fired Power Plant in Deep Eutectic Solvents

Energies ◽  
2020 ◽  
Vol 13 (2) ◽  
pp. 438
Author(s):  
Kyle McGaughy ◽  
M. Toufiq Reza
Keyword(s):  
Power Plant ◽  
Ethylene Glycol ◽  
Flue Gas ◽  
Density Functional ◽  
Choline Chloride ◽  
Deep Eutectic Solvents ◽  
Pulverized Coal ◽  
Molar Ratio ◽  
Modeling Framework ◽  
So2 Capture

In this study, CO2 and SO2 captures from post-combustion flue gas from a pulverized coal-fired power plant were evaluated using deep eutectic solvents (DES) to replace existing mono-ethanol amine (MEA) and CanSolv technologies. The system design of the DES-based CO2 and SO2 capture was based on the National Energy Technology Laboratory’s (NETL) 550 MWe pulverized coal-fired power plant model using Illinois #06 coal. Two of the most studied DES (choline chloride and urea at a 1:2 molar ratio and methyltriphenylphosphonium bromide (METPB) and ethylene glycol at a 1:3 molar ratio) for CO2 and SO2 capture were evaluated for this system analysis. Physical properties of DES were evaluated using both density functional theory (DFT)-based modeling as well as with documented properties from the literature. A technoeconomic assessment (TEA) was completed to assess DES ability to capture CO2 and SO2. Both solvents were able to fully dissolve and capture all SO2 present in the flue gas. It was also found from the system analyses that choline chloride and urea outperformed METPB and ethylene glycol (had a lower final cost) when assessed at 10–30% CO2 capture at high operating pressures (greater than 10 bar). At high system sizes (flow rate of greater than 50,000 kmoles DES per hour), choline chloride:urea was more cost effective than METPB:ethylene glycol. This study also establishes a modeling framework to evaluate future DES for physical absorption systems by both thermophysical and economic objectives. This framework can be used to greatly expedite DES candidate screening in future studies.

scholarly journals A density functional theory study of the adsorption of uracil on the Au(100) surface

2011 ◽  
Vol 467 (2131) ◽  
pp. 1959-1969 ◽  
Author(s):  
Simona Irrera ◽  
Nora H. de Leeuw
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Rational Design ◽  
Molecular Level ◽  
Gold Surface ◽  
Functional Theory ◽  
Enol Tautomer ◽  
Experimental Findings ◽  
Adsorbate Structure ◽  
Insight Into

We have used plane-wave density functional theory methods to explore the adsorption modes and configurations of uracil molecules on a gold surface to gain insight into the rational design of surface functionalization. We have investigated at the molecular level, the interactions of the RNA pyrimidine base uracil molecule isolated on the single crystal (100) surface of the gold substrate to determine the structure of uracil and orientation. Our calculations have shown that the most stable adsorbate structure is the enol tautomer of uracil, which adsorbs flat onto the gold surface through one of its carbonyl atoms. This configuration, which is compatible with previous experimental findings, is thermodynamically preferred over the adsorbed keto structure by approximately 0.23 eV (22.2 kJ mol −1 ).

High-Entropy Alloys as Catalysts for the CO2 and CO Reduction Reactions

2019 ◽  
Author(s):  
Jack Pedersen ◽  
Thomas Batchelor ◽  
Alexander Bagger ◽  
Jan Rossmeisl
Keyword(s):  
Density Functional ◽  
Rational Design ◽  
Hydrogen Adsorption ◽  
Co Adsorption ◽  
Reduction Reaction ◽  
Supervised Machine Learning ◽  
High Entropy Alloys ◽  
High Entropy ◽  
Co Reduction ◽  
Disordered Alloy

Using the high-entropy alloys (HEAs) CoCuGaNiZn and AgAuCuPdPt as starting points we provide a framework for tuning the composition of disordered multi-metallic alloys to control the selectivity and activity of the reduction of carbon dioxide (CO2) to highly reduced compounds. By combining density functional theory (DFT) with supervised machine learning we predicted the CO and hydrogen (H) adsorption energies of all surface sites on the (111) surface of the two HEAs. This allowed an optimization for the HEA compositions with increased likelihood for sites with weak hydrogen adsorption{to suppress the formation of molecular hydrogen (H2) and with strong CO adsorption to favor the reduction of CO. This led to the discovery of several disordered alloy catalyst candidates for which selectivity towards highly reduced carbon compounds is expected, as well as insights into the rational design of disordered alloy catalysts for the CO2 and CO reduction reaction.

scholarly journals H2O coordination in macropa complexes of f elements (Ac, La, Lu): feasibility of the 11th coordination site

2021 ◽  
Author(s):  
Attila Kovács ◽  
Zoltán Varga
Keyword(s):  
Aqueous Solution ◽  
Metal Ion ◽  
Density Functional ◽  
Molecular Level ◽  
Density Functional Theory Calculations ◽  
Functional Theory ◽  
Coordination Site ◽  
Additional Ligand ◽  
Ligand Coordination ◽  
Bonding Properties

AbstractThe feasibility of an additional ligand coordination at the 11th coordination site of actinium, lanthanum, and lutetium ions in 10-fold coordinated macropa complexes has been studied by means of density functional theory calculations. The study covered the two main macropa conformers, Δ(δλδ)(δλδ) and Δ(λδλ)(λδλ), favoured by larger (Ac3+, La3+) and smaller (Lu3+) ions, respectively. At the molecular level, the coordination of H2O is the most favourable to the largest Ac3+ while only slightly less to La3+. Protonation of the picoline arms enhances the coordination by shifting the metal ion closer to the open site of the ligand. The choice of macropa conformer has only a slight influence on the strength and bonding properties of the H2O coordination. Aqueous solution environment decreases considerably the energy gain of H2O coordination at the 11th coordination site.

In situ nanoscale visualization of solvent effects on molecular crystal surfaces

CrystEngComm ◽  
2021 ◽  
Author(s):  
Mikkel Herzberg ◽  
Anders Støttrup Larsen ◽  
Tue Hassenkam ◽  
Anders Østergaard Madsen ◽  
Jukka Rantanen
Keyword(s):  
Solid Solution ◽  
Solvent Effects ◽  
Molecular Crystal ◽  
Rational Design ◽  
Molecular Level ◽  
Molecular Crystals ◽  
Crystal Surfaces ◽  
Solution Interface ◽  
Atomic Force

Solvents can dramatically affect molecular crystals. Obtaining favorable properties for these crystals requires rational design based on molecular level understanding of the solid-solution interface. Here we show how atomic force...

POSSIBILITY OF MOLECULAR-SWITCH WITH CONTROLLED HYDROGEN BOND: UTILITY OF COMBINATION OF 2,2′-BIIMIDAZOLE AND REDOX-ACTIVE LIGAND

2005 ◽  
Vol 04 (01) ◽  
pp. 333-344 ◽  
Author(s):  
HIROTOSHI MORI ◽  
EISAKU MIYOSHI
Keyword(s):  
Density Functional ◽  
Molecular Level ◽  
Molecular Switch ◽  
Vibration Band ◽  
Functional Theory ◽  
Inorganic Molecule ◽  
Redox Active Ligand ◽  
Active Ligand ◽  
Redox Active ◽  
Stretching Vibration

A new inorganic molecule [ Co(Hbim) ( C 6 H 4 O 2)( NH 3)2]2 that can be used as a new optically durable molecular switch was theoretically designed in the framework of density functional theory. Three stable minima, belonging to 1 A g , 5 A 1, and 9 A g states, were found in the complex. Theoretically predicted infrared spectra of the complexes showed that a strong peak of NH stretching vibration is observed at 2690, 2120, and 2770 cm -1 in the 1 A g , 5 A 1, and 9 A g states, respectively. The apparent red shift of the NH stretching vibration band in the 5 A 1 state make it possible to distinguish the electronic state from others (1 A g and 9 A g ). This means that the complex can be used as a molecular level switch whose memory can be stably read by IR light without any photoreaction process; namely, without memory degradation.

Rational Design of Novel Materials From Polymer Microrheology

2010 ◽  
Author(s):  
Rodrigo E. Teixeira ◽  
Richard S. Graham
Keyword(s):  
Rational Design ◽  
Molecular Level ◽  
Pressure Vessels ◽  
Novel Materials ◽  
Entangled Polymers ◽  
Stochastic Fluctuations ◽  
Safety Margins ◽  
Polymer Liquids ◽  
Entangled Polymer ◽  
High Degree

The visco-elastic properties of entangled polymer liquids arise from molecular-scale topological interactions and stochastic fluctuations under flow. Here, the evolutions of individual entangled polymers were observed in rheologically relevant shear flow histories. We uncover a high degree of molecular individualism and broad conformational distributions resulting from incessant stretch-collapse cycles. The data and insights of the present study may lead to improved molecular-level models and constitutive equations. These tools, in turn, may enable the rational design of novel materials with properties tailored to accomplish specific tasks such as high-pressure vessels and piping with greater safety margins and cost-effectiveness.

scholarly journals Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Panlong Zhai ◽  
Mingyue Xia ◽  
Yunzhen Wu ◽  
Guanghui Zhang ◽  
Junfeng Gao ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Water Splitting ◽  
Layered Double Hydroxide ◽  
Hydrogen Evolution Reaction ◽  
Active Sites ◽  
Density Functional ◽  
Rational Design ◽  
Single Atom ◽  
Nickel Iron ◽  
Double Hydroxide

AbstractRational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru1/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru1/D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm−2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru1/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O–O coupling at a Ru–O active site for oxygen evolution reaction. The Ru1/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts.

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