Capture of Carbonyl Sulfide by Organic Liquid Mixtures: A Systematic DFT Investigation

Abduesslam, Mahmoud; Kayı, Hakan

doi:10.1021/acs.iecr.0c04752

Cited by 9 publications

(3 citation statements)

References 35 publications

(94 reference statements)

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“…TS‐b and Prod‐b have been located and are displayed in Figure 4. In this process, the O2 atom of the hydroxyl moiety performs the nucleophilic attack on the C1 of COS to form the O2‐C1 bond, [ 15 ] along with H1 transferred from O2 to N1. The calculated energy profile is listed in Figure 5.…”

Section: Resultsmentioning

confidence: 99%

“…In their work, the structures of reactants, transition states, and products were examined to explain the COS hydrolysis mechanism. Kayi and Abduesslam [ 15 ] carried out a systematic DFT investigation of COS and organic liquid mixtures of amines and alcohols. However, up to now, the theoretical calculation of COS removal by an aqueous MDEA solution has not been reported yet.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

The capture of carbonyl sulfide by N‐methyldiethanolamine: A systematic density functional theory investigation

Xue¹,

Liao

Li³

et al. 2022

J Chinese Chemical Soc

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In this contribution, the mechanism of carbonyl sulfide (COS) absorption by N‐methyldiethanolamine (MDEA) aqueous solution was explored via theoretical computations. Detailed reaction mechanisms were analyzed using density functional theory (DFT) calculations at the B3LYP‐D3 level of theory. In total, four different pathways for COS absorption by MDEA have been considered. The most favorable pathway for the removal of COS is a three‐step mechanism including the hydrolysis, proton transfer, and dissociation of CO2, and hydrolysis is the rate‐determining step. The mechanisms of the COS absorption by different amines were investigated, and the calculated results suggest that the total energy barrier for the COS absorption by MDEA is comparable to that by monoethanolamine (MEA), diethanolamine (DEA), and diisopropylamine (DIPA), indicating the COS absorption by all the four amines are feasible, while MDEA gives a better performance in terms of thermodynamics.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

The capture of carbonyl sulfide by N‐methyldiethanolamine: A systematic density functional theory investigation

Xue¹,

Liao

Li³

et al. 2022

J Chinese Chemical Soc

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show abstract

“…Earlier researches have indicated the significant influences of molecular structures of alkanolamines on the reaction rates of COS . Therefore, more investigations were focused on the exploration of candidate compounds with largely enhanced reaction rates with COS from the vast chemical space. − …”

Section: Introductionmentioning

confidence: 99%

Unveiling the Quantitative Relationships between Electron Distribution and Steric Hindrance of Organic Amines and Their Reaction Rates with Carbonyl Sulfur: A Theoretical Calculation Investigation

Liu,

Chen,

Guo

et al. 2023

J. Phys. Chem. A

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The removal of carbonyl sulfide (COS) commonly contained in natural gas is of great significance but still very challenging via a widely employed absorption process due to its low reactivity and solubility in various commercial solvents. Artificial intelligence (AI) is playing an increasingly important role in the exploration of desulfurization solvents. However, practically feasible AI models still lack a thorough understanding of the reaction mechanisms. Machine learning (ML) models established on chemical mechanisms exhibit enhanced chemical interpretability and prediction performance. In this study, we constructed a series of solvent molecules with varying functional groups, including linear aliphatic amines, cyclic aliphatic amines, and aromatic amines and proposed a three-step reaction pathway to dissect the effects of charge and steric hindrance of different substituents on their reaction rates with COS. Chemical descriptors, based on electrostatic potential (ESP), average local ionization energy (ALIE) theory, Hirshfeld charges, and Fukui functions, were used to correlate and predict the electrophilic reactivity of amine groups with COS. Substituents influence the reaction rate by changing the attraction interaction of amine groups to COS molecules and the electron rearrangement in the electrophilic reaction. Furthermore, they have more pronounced steric effects on the reaction rate in the linear amines. The descriptors N_ALIE and q(N) were found to be crucial in predicting the reactivity of amine groups with COS. Present study provides a comprehensive understanding of the reaction mechanisms of COS with amine compounds, offers specific chemical principles for the development of chemistry-driven ML models, sheds light on other types of electrophilic reactions occurring on amine and phosphine groups, and guides the development of chemical solvents in gas absorption processes.

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Boosting catalytic hydrolysis of carbonyl sulfide over K+ modified CeO2 nanospheres at low-temperature

Xiong,

Gong,

et al. 2024

Applied Surface Science

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Capture of Carbonyl Sulfide by Organic Liquid Mixtures: A Systematic DFT Investigation

Cited by 9 publications

References 35 publications

The capture of carbonyl sulfide by N‐methyldiethanolamine: A systematic density functional theory investigation

The capture of carbonyl sulfide by N‐methyldiethanolamine: A systematic density functional theory investigation

Unveiling the Quantitative Relationships between Electron Distribution and Steric Hindrance of Organic Amines and Their Reaction Rates with Carbonyl Sulfur: A Theoretical Calculation Investigation

Boosting catalytic hydrolysis of carbonyl sulfide over K+ modified CeO2 nanospheres at low-temperature

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