Sterically Hindered Amine-Based Absorbents for the Removal of CO<sub>2</sub> from Gas Streams

Bougie, Francis; Iliuta, Maria C.

doi:10.1021/je200731v

Cited by 136 publications

(81 citation statements)

References 171 publications

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“…In the design problem, the algorithm used 73 can rapidly evaluate around 200,000 molecular structures to generate the few tens of solvents comprising the "long list". Solvents are designed and/or evaluated using GC and non-GC-based models for the prediction of properties that are specifically selected to reflect the major driving forces for CO 2 capture. The selected properties provide a set of solvent performance measures that link the chemical structure of the solvent to thermodynamic, reactivity and sustainability characteristics of importance in the capture/regeneration process (see section 3 for details).…”

Section: Stage 1 Of the Methodologymentioning

confidence: 99%

“…The final specification required to enable the application of our approach to CO 2 (Table E1 in Supporting Information), serves as a benchmark to assess the viability of the new capture solvents proposed in our work and to assess the potential performance improvements; secondly, the Commercial class (C) containing 101 acyclic, aliphatic amines for which we had limited or no knowledge regarding their suitability as CO 2 capture solvents, prior to this work (Tables E2, E3 and E4 in Supporting Information). The C-class solvents are assumed to be commercially available because they were retrieved from public and commercial databases.…”

Section: The Molecular Search Spacementioning

confidence: 99%

“…The results are shown in Table 10. Table 10-Isomers corresponding to structures of Table 9 based on Structure-Property Relations (1) and (2). IUPAC names have been assigned using Marvin 6.0.5 86 .…”

Section: Stage 2 Of Solvent Designmentioning

confidence: 99%

“…Puxty et al 18 Yamada et al 19 Tontiwachwuthikul et al 12 Hydroxylamines 2-4 carbons between hydroxyl and amine functional groups increase absorption capacity. (2) Singh and Versteeg 10 Aronu et al 20 …”

Section: Introductionmentioning

confidence: 99%

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Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

Παπαδόπουλος

Badr

Chremos

et al. 2016

Mol. Syst. Des. Eng.

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We propose a Computer Aided Molecular Design (CAMD) method which employs optimization to support the synthesis and selection of high performance molecules for use in process systems and to guide experimental efforts. The method can be used to address challenging applications where a) the desired molecules exhibit phase and chemical equilibrium, b) numerous combinations of molecules need to be evaluated, and c) multiple criteria must be considered to capture the effects of molecular chemistry on the process system performance. The method is applied to the design of solvents in chemical absorption processes for the separation of carbon dioxide (CO 2 ) from gas streams. The molecular design problem is first approached via a fast screening stage where molecules are evaluated based on the simultaneous consideration of multiple performance indices pertaining to thermodynamics, reactivity and sustainability. A few high-performance solvents are further evaluated using an advanced group contribution equation of state to predict reliably the highly non-ideal equilibrium behavior of solvent-water-CO 2 mixtures. Several promising novel solvents for CO 2 capture are proposed and can now be assessed experimentally. The proposed method can readily be applied to other chemical absorption processes to accelerate the identification of novel solvents. AbstractThe identification of improved carbon dioxide (CO 2 ) capture solvents remains a challenge due to the vast number of potentially-suitable molecules. We propose an optimization-based computer-aided molecular design (CAMD) method to identify and select, from hundreds of thousands of possibilities, a few solvents of optimum performance for CO 2 chemisorption processes, as measured by a comprehensive set of criteria. The first stage of the approach consists in a fast screening stage where solvent structures are evaluated based on the simultaneous consideration of important pure component properties reflecting thermodynamic, kinetic, and sustainability behaviour. The impact of model uncertainty is considered through a systematic method that employs multiple models for the prediction of performance indices. In a second stage, high-performance solvents are further selected and evaluated using a more detailed thermodynamic model, namely the group-contribution statistical associating fluid theory for square well potentials (SAFT-γ SW), to predict accurately the highly non-ideal chemical and phase equilibrium of the solvent-water-CO 2 mixtures. The proposed CAMD method is applied to the design of novel molecular structures and to the screening of a dataset of commercially available amines. New molecular structures and commercially-available compounds that have received little attention as CO 2 capture solvents are successfully identified and assessed using the proposed approach. We recommend that these solvents given priority in experimental studies to identify new compounds.

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Section: Stage 1 Of the Methodologymentioning

confidence: 99%

Section: The Molecular Search Spacementioning

confidence: 99%

Section: Stage 2 Of Solvent Designmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

Παπαδόπουλος

Badr

Chremos

et al. 2016

Mol. Syst. Des. Eng.

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“…It is defined, based on molecular structure, as a primary amine in which the amino group is attached to a tertiary carbon or a secondary amine in which the amino group is attached to at least one secondary or tertiary carbon [2], [3]. Due to the hindrance produced by the bulky group adjacent to its amino group, a sterically hindered amine forms unstable carbamate with CO 2 .…”

Section: Introductionmentioning

confidence: 99%

Heat Capacities of Aqueous Ternary Mixtures of 2-Amino-2-Methyl-1, 3-Propanediol + Piperazine or Lithium Bromide

Olivia¹,

Leron²,

Li³

2014

IJCEA

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Abstract-In this work, we reported the molar heat capacities, C P , of aqueous solutions of the sterically hindered amines 2-amino-2-methyl-1, 3-propanediol (AMPD), and its aqueous ternaries containing piperazine (PZ) or lithium bromide (LiBr). Measurements were performed in the temperature range 303.15 K to 353.15 K and atmospheric pressure by heat flow differential scanning calorimetry. The excess molar heat capacities, C P E , of the binary solutions were determined, and the data were represented as function of temperature and composition using a RedlichKister-type equation. The C P of the ternary mixtures was correlated with temperature and amine concentration using the Sohnel and Novotny equation. Results showed that the calculated data agree very well with experimental C P values at average absolute deviation values of less than 0.2%. Index Terms-2-amino-2-methyl-1, 3-propanediol, molar heat capacity, redlichkister equation, sohnel and novotny equation.

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An experimental/computational study of steric hindrance effects on CO₂ absorption in (non)aqueous amine solutions

et al. 2022

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The reaction kinetics and molecular mechanisms of CO 2 absorption using nonaqueous and aqueous monoethanolamine (MEA)/methyldiethanolamine (MDEA)/2-amino-2-methy-1-propanol (AMP) solutions were analyzed by the stopped-flow technique and ab initio molecular dynamics (AIMD) simulations. Pseudo first-order rate constants (k 0 ) of reactions between CO 2 and amines were measured. A kinetic model was proposed to correlate the k 0 to the amine concentration, and was proved to perform well for predicting the relationship between k 0 and the amine concentration. The experimental results showed that AMP/MDEA only took part in the deprotonation of MEA-zwitterion in nonaqueous MEA + AMP/MEA + MDEA solutions. In aqueous solutions, AMP can also react with CO 2 through base-catalyzed hydration mechanism beside the zwitterion mechanism. Molecular mechanisms of CO 2 absorption were also explored by AIMD simulations coupled with metadynamics sampling. The predicted free-energy barriers of key elementary reactions verified the kinetic model and demonstrated the different molecular mechanisms for the reaction between CO 2 and AMP.

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Sterically Hindered Amine-Based Absorbents for the Removal of CO₂ from Gas Streams

Cited by 136 publications

References 171 publications

Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

Heat Capacities of Aqueous Ternary Mixtures of 2-Amino-2-Methyl-1, 3-Propanediol + Piperazine or Lithium Bromide

An experimental/computational study of steric hindrance effects on CO₂ absorption in (non)aqueous amine solutions

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Sterically Hindered Amine-Based Absorbents for the Removal of CO2 from Gas Streams

Cited by 136 publications

References 171 publications

Computer-aided molecular design and selection of CO2 capture solvents based on thermodynamics, reactivity and sustainability

Computer-aided molecular design and selection of CO2 capture solvents based on thermodynamics, reactivity and sustainability

Heat Capacities of Aqueous Ternary Mixtures of 2-Amino-2-Methyl-1, 3-Propanediol + Piperazine or Lithium Bromide

An experimental/computational study of steric hindrance effects on CO2 absorption in (non)aqueous amine solutions

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Product

Resources

About

Sterically Hindered Amine-Based Absorbents for the Removal of CO₂ from Gas Streams

Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

Computer-aided molecular design and selection of CO₂ capture solvents based on thermodynamics, reactivity and sustainability

An experimental/computational study of steric hindrance effects on CO₂ absorption in (non)aqueous amine solutions