New Amines for CO<sub>2</sub> Capture. III. Effect of Alkyl Chain Length between Amine Functions on Polyamines Degradation

Lepaumier, Hélène; Martin, Sandrine; Picq, Dominique; Delfort, Bruno; Carrette, Pierre-Louis

doi:10.1021/ie902006a

Cited by 92 publications

(85 citation statements)

References 24 publications

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“…Among these, solid adsorbents have been commonly fit for the integrated gasification combined cycles (IGCC) related pre-combustion CO 2 capture processes [4,5], e.g., sorption enhanced water gas shift (SEWGS) and sorption enhanced biomass reforming (SEBR) reactions [12][13][14][15]. Among the abundant solid adsorbents which tend to capture CO 2 at moderate temperatures [5,[14][15][16], layered double hydroxides (LDHs) derived metal oxides [17][18][19][20][21] and magnesium oxide (MgO) based compounds [22][23][24][25][26] are promising for the SEWGS and SEBR technologies in the temperature range of 200-400 • C [10,[27][28][29][30]. LDHs have the reputation of outstanding thermal stability and relatively fast CO 2 adsorption kinetics.…”

Section: Introductionmentioning

confidence: 99%

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

et al. 2017

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Abstract:In this work, we report on a novel sodium dodecyl sulfate (SDS)-assisted magnesium oxide (MgO)-based porous adsorbent synthesized by hydrothermal method for intermediate CO 2 capture. For industrial MgO, its CO 2 adsorption capacity is normally less than 0.06 mmol g −1 , with a specific surface area as low as 25.1 m 2 g −1 . Herein, leaf-like MgO nanosheets which exhibited a disordered layer structure were fabricated by the introduction of SDS surfactants and the control of other synthesis parameters. This leaf-like MgO adsorbent showed an excellent CO 2 capacity of 0.96 mmol g −1 at moderate temperatures (~300 • C), which is more than ten times higher than that of the commercial light MgO. This novel mesoporous MgO adsorbent also exhibited high stability during multiple CO 2 adsorption/desorption cycles. The excellent CO 2 capturing performance was believed to be related to its high specific surface area of 321.3 m 2 g −1 and abundant surface active adsorption sites. This work suggested a new synthesis scheme for MgO based CO 2 adsorbents at intermediate temperatures, providing a competitive candidate for capturing CO 2 from certain sorption enhanced hydrogen production processes.

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Section: Introductionmentioning

confidence: 99%

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

et al. 2017

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“…It is therefore important to consider these issues at early stage. Lately there have been several systematic degradation studies conducted to review how molecular structure influences different types of degradation (Lepaumier et al 2009a(Lepaumier et al , 2009b(Lepaumier et al , 2010Eide-Haugmo 2011;Vevelstad et al 2013a). …”

Section: Introductionmentioning

confidence: 99%

Extensive dataset for oxidative degradation of ethanolamine at 55–75°C and oxygen concentrations from 6 to 98%

Vevelstad

Johansen

Knuutila

et al. 2016

International Journal of Greenhouse Gas Control

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Post combustion CO2 capture using amines as chemical absorbents is a relatively mature technology. Rate of reaction and desorption energy demand are normally prime criteria for evaluation of new solvents while degradation and corrosion studies are often postponed. However, degradation and corrosion are in many cases showstoppers and should be considered at an early stage. In this work, a systematic study has been conducted on oxidative degradation of 30 wt% ethanolamine (MEA) for oxygen concentrations: 6, 21, 49 and 98% and temperatures: 55, 65 and 75 °C. The formation of ten primary degradation compounds (acids, ammonia and alkyl amines) and seven secondary degradation compounds (HEGly, OZD, HEPO, HEF, HEA, HEI and BHEOX was monitored as function of time over a period of 3 -6 weeks. The full comprehensive data set is available in the supplementary information for development of models describing the degradation behavior. Suggested mechanisms for formation of seven secondary degradation compounds; HEGly, HEPO, OZD, HEF, HEA, BHEOX and HEI from literature were compiled and discussed in view of the experimental results to suggest pathways which are more likely than others.The rate of MEA degradation increases with increasing temperature and oxygen concentration. The overall nitrogen balances were closed within 83-97%; the higher deviations observed at the highest temperature, 75 o C. HEF, HEI and ammonia were the degradation compounds that most significantly contributed to the nitrogen balance in most experiments. However, at 6% O2 content, HEGly was the major nitrogen containing degradation compound identified. Formate was found to be the major anionic compound in all experiments.HEGly formation was found to be independent on O2 partial pressure, but this may not be true for the further reaction of HEGly. The results suggests OZD formation to be oxygen dependent. However, only one mechanism is so far suggested for an oxygen dependent pathway. Both OZD and HEPO concentrations increase with oxygen concentration. Separate laboratory experiments at constant temperature (55-75 o C) do not capture the HEPO formation seen in pilot plant samples indicating that higher temperatures and/or temperature cycles are necessary.The results clearly show that performing accelerated degradation tests with 98% oxygen cannot easily be extrapolated to what happens at 6% oxygen, and therefore may not be representative for the situation in an industrial plant both with regard to rates of formation and products formed.

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“…The models typically used in chemisorption process design, while of high accuracy, are specific to a given solvent and require extensive experimental data on each solvent to be studied; this is the case of models of the thermodynamics and kinetics of aqueous alkanolamine and CO 2 mixtures (e.g., eNRTL models [36][37][38], and of the kinetics of degradation reactions [39][40][41] . Few predictive models that relate solvent molecular structure or solvent blend composition to properties, and hence performance, are available to support CAMD activities.…”

Section: Diaminesmentioning

confidence: 99%

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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New Amines for CO₂ Capture. III. Effect of Alkyl Chain Length between Amine Functions on Polyamines Degradation

Cited by 92 publications

References 24 publications

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

Extensive dataset for oxidative degradation of ethanolamine at 55–75°C and oxygen concentrations from 6 to 98%

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

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New Amines for CO2 Capture. III. Effect of Alkyl Chain Length between Amine Functions on Polyamines Degradation

Cited by 92 publications

References 24 publications

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

Hydrothermal Fabrication of High Specific Surface Area Mesoporous MgO with Excellent CO2 Adsorption Potential at Intermediate Temperatures

Extensive dataset for oxidative degradation of ethanolamine at 55–75°C and oxygen concentrations from 6 to 98%

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

Contact Info

Product

Resources

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New Amines for CO₂ Capture. III. Effect of Alkyl Chain Length between Amine Functions on Polyamines Degradation

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