Influence of experimental setup on amine degradation

Vevelstad, Solrun Johanne; Grimstvedt, Andreas; Knuutila, Hanna; Silva, Eirik Falck da; Svendsen, Hallvard F.

doi:10.1016/j.ijggc.2014.06.028

Cited by 29 publications

(34 citation statements)

References 28 publications

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“…HEPO is considered to be an end product. Another formation reaction was also suggested by Gouedard (Gouedard 2014) where HEGly is formed from HEHEAA and not the other way around as earlier suggested and supported by mixing experiments (da Silva et al 2012;Vevelstad et al 2014a). It is likely that several of these mechanisms occur in a plant, and which ones are the more favorable could be supported using molecular modelling (Gupta et al 2014).…”

Section: Hegly Hepo and Ozdmentioning

confidence: 61%

“…The molecules were converted to ions using electrospray ionization (MEA, LC-MS mix, alkyl amine and ammonia) or atmospheric-pressure chemical ionization (nitrosamine). Mobile phases and columns used are described by (Lepaumier et al 2011a,b;da Silva et al 2012;Vevelstad et al 2013b;Vevelstad et al 2014a). The system used for analyses of anions was an ICS-5000 Dual RFIC Ion Chromatography Dionex System.…”

Section: Set-up and Analytical Methodologymentioning

confidence: 99%

“…The reaction scheme in Figure 11 shows all suggested mechanisms for the formation of HEGly and the two isomers of HEPO as well as the formation of other products from HEGly. F1 means that the reaction pathway is suggested by (Gouedard 2014), F2 by (da Silva et al 2012), F3 by (Strazisar et al 2003) and F4 by (Vevelstad et al 2014a). To summarize, two formation reactions are suggested for HEGly and 6 reactions consuming HEGly.…”

Section: Hegly Hepo and Ozdmentioning

confidence: 95%

“…The first step is formation of N-(2-hydroxyethyl)-2-[(2-hydroxyethyl)amino]-acetamide (HEHEAA) (da Silva et al 2012) and the second step cyclisation of HEHEAA with loss of water (Strazisar et al 2003;da Silva et al 2012). Recently several new mechanisms have been suggested for the formation of both HEGly and the two isomers of HEPO (1HEPO -1-(2-hydroxyethyl)-2-piperazinone/59702-23-7 & 4HEPO -4-(2-hydroxyethyl)-2-piperazinone/ 23936-04-1 (Gouedard 2014;Vevelstad et al 2014a)). For one of the mechanism OZD plays an important role together with HEGly for the formation of HEPO.…”

Section: Hegly Hepo and Ozdmentioning

confidence: 99%

“…The primary degradation compounds usually take part in the formation of several secondary products and in some cases there are several mechanisms suggested in the literature for the same degradation compounds, e.g. HEPO (Strazisar et al 2003;da Silva et al 2012;Gouedard 2014) and HEGly (Gouedard 2014;Vevelstad et al 2014a).…”

Section: Introductionmentioning

confidence: 99%

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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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Section: Hegly Hepo and Ozdmentioning

confidence: 61%

Section: Set-up and Analytical Methodologymentioning

confidence: 99%

Section: Hegly Hepo and Ozdmentioning

confidence: 95%

Section: Hegly Hepo and Ozdmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

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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View full text Add to dashboard Cite

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Uncertainties in Modelling the Environmental Impact of Solvent Loss through Degradation for Amine Screening Purposes in Post‐combustion CO₂Capture

Badr

Papadokonstantakis

Bennett

et al. 2017

Process Systems and Materials for CO2 Capture

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Modeling of Oxidative MEA Degradation

et al. 2014

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Considerable amount of work had been recently done researching the degradation of solvents for CO 2 post combustion capture, especially for the benchmark solvent MEA. The degradation of the solvent can cause plant corrosion and losses in the process performance since the solvent might loses its capacity to absorb CO 2 . Thus, a better understanding of this phenomena is important for the overall process performance. Oxidative degradation is likely to occur at absorber conditions due to the presence of oxygen in the flue gas. Differently from the thermal degradation, the oxidative degradation is not well understood. This work presents a preliminary attempt to rigorously model the degradation of solvents for CO 2 capture. Experimental data available in the literature were used to regress some of the model parameters. Several assumptions had to be made due to the lack of knowledge. The model, however, does a reasonable job of representing the dynamic trends of the oxidative degradation in the MEA system. This model is still under further development and new components, experiments and reactions are being implemented in the model.

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Influence of experimental setup on amine degradation

Cited by 29 publications

References 28 publications

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

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

Uncertainties in Modelling the Environmental Impact of Solvent Loss through Degradation for Amine Screening Purposes in Post‐combustion CO₂Capture

Modeling of Oxidative MEA Degradation

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Influence of experimental setup on amine degradation

Cited by 29 publications

References 28 publications

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

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

Uncertainties in Modelling the Environmental Impact of Solvent Loss through Degradation for Amine Screening Purposes in Post‐combustion CO2Capture

Modeling of Oxidative MEA Degradation

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Product

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Uncertainties in Modelling the Environmental Impact of Solvent Loss through Degradation for Amine Screening Purposes in Post‐combustion CO₂Capture