Computational Modeling and Simulation of CO<sub>2</sub> Capture by Aqueous Amines

Yang, Xin; Rees, Robert J.; Conway, William; Puxty, Graeme; Yang, Qi; Winkler, David A.

doi:10.1021/acs.chemrev.6b00662

Cited by 153 publications

(117 citation statements)

References 509 publications

(904 reference statements)

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“…Thus, CO 2 emission control is imperative by the Paris Climate Accord 5,6 . Chemisorption is the most selective and thus promising technology for capturing CO 2 emitted from fossil flue gas due to its simplicity and unique flexibility in dealing with wide concentrations and volumes of CO 2 -containing gases 7–9 . However, its shortcomings are also obvious, including slow sorption and desorption rates.…”

Section: Introductionmentioning

confidence: 99%

Catalyst-TiO(OH)2 could drastically reduce the energy consumption of CO2 capture

et al. 2018

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Implementing Paris Climate Accord is inhibited by the high energy consumption of the state-of-the-art CO2 capture technologies due to the notoriously slow kinetics in CO2 desorption step of CO2 capture. To address the challenge, here we report that nanostructured TiO(OH)2 as a catalyst is capable of drastically increasing the rates of CO2 desorption from spent monoethanolamine (MEA) by over 4500%. This discovery makes CO2 capture successful at much lower temperatures, which not only dramatically reduces energy consumption but also amine losses and prevents emission of carcinogenic amine-decomposition byproducts. The catalytic effect of TiO(OH)2 is observed with Raman characterization. The stabilities of the catalyst and MEA are confirmed with 50 cyclic CO2 sorption and sorption. A possible mechanism is proposed for the TiO(OH)2-catalyzed CO2 capture. TiO(OH)2 could be a key to the future success of Paris Climat e Accord.

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Section: Introductionmentioning

confidence: 99%

Catalyst-TiO(OH)2 could drastically reduce the energy consumption of CO2 capture

et al. 2018

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“…We here use a representative subset of four alkanolamine compounds; the well-characterized monoethanolamine (MEA) as a standard and benchmark, and three representatives for each classification of amines: a primary amine 3-aminopropanol (MPA), a secondary amine 2-methylaminoethanol (MMEA) and a tertiary amine 4-diethylamino-2-butanol (DEAB), see Figure 1. Molecular simulations are able to provide detailed insight into liquid solution behavior and to calculate relevant compound-specific thermodynamic and transport properties, for novel CO 2 absorbing compounds 8 , some of which are not available in the literature and not accessible experimentally. For example, the diffusion coefficients of CO 2 in these absorptive alkanolamine solvents are not possible to measure experimentally because of the high reactivity in the amine solution.…”

Section: Introductionmentioning

confidence: 99%

Solvation and Dynamics of CO₂ in Aqueous Alkanolamine Solutions

Melnikov

Stein

2018

ACS Sustainable Chem. Eng.

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Carbon dioxide sequestration from flue gases by chemical absorption is the most versatile process.The molecular engineering of novel high-performant biogas upgrading alkanolamine compounds requires detailed information about their properties in mixed solution. The liquid structure properties of four representative alkanolamine molecules (monoethanolamine (MEA) as a reference and standard, 3-aminopropanol (MPA), 2-methylaminoethanol (MMEA) and 4-diethylamino-2butanol (DEAB)) in the presence of CO 2 were investigated over a wide range of solvent alkanolamine/water mixture compositions and temperature. In aqueous solution, for the alkanolamine molecules MEA, MPA and MMEA hydrogen bonding with solvent water molecules is dominating over CO 2 interactions. Analysis of the liquid structure reveals that carbon dioxide shows no preference of approaching the alkanolamine but is rather displaced by water molecules as the water content increases. CO 2 dissolved in aqueous DEAB, however, accumulates within clusters of DEAB molecules almost devoid of water. The calculated carbon dioxide diffusion coefficients for all four molecules agree well with experiment where available and are obtained for all mixture compositions and as a function of temperature. The solute diffusion correlates with the mobility of the alkanolamines in water at various ternary mixture compositions. Kinetic aspects of the CO 2alkanolamine interactions are described by characteristic residence times of CO 2 . The hydrophobic interaction of carbon dioxide with the alkanolamine has a lifetime of the order of tens of picoseconds whereas polar interactions are about one order of magnitude shorter. The tertiary amine DEAB displays many favorable features for an efficient CO 2 chemisorption process. Molecular engineering of novel compounds for absorptive sequestration has to take into account not only the thermodynamics and chemical reactivity but also liquid structure properties, the dynamics of CO 2 diffusion and the kinetics of interactions in complex ternary solutions.

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“…7 Although feasibility studies indicate that it will remain competitive in the future, this technology suffers from many problems, such as high cost, toxicity, degradation, and evaporation of the solvent. Yang et al 8 discuss the use of quantum mechanical methods to model the reactions at the basis of CO 2 capture by aqueous amines, pointing out the merits of the different mechanisms. A critical review of the influence of the simulation parameters and solvent models on the accuracy and reliability of the results is also presented to give a perspective on the capability for in silico design of more effective systems.…”

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confidence: 99%