A new test rig for studies of degradation of CO2 absorption solvents at process conditions; comparison of test rig results and pilot plant data for degradation of MEA

Einbu, Aslak; DaSilva, Eirik; Haugen, Geir; Grimstvedt, Andreas; Lauritsen, K.; Zahlsen, Kolbjørn; Vassbotn, Terje

doi:10.1016/j.egypro.2013.05.160

Cited by 31 publications

(50 citation statements)

References 3 publications

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“…Some of the newer experiments, B4 (65 °C -98% O2), B2-I (65 °C -21% O2, run1), B2-II (65 °C -21% O2 run2) and A2-III (55 °C -21% O2, run3), were analyzed for NDELA and NHEGly. NHEGly was observed in higher amounts than NDELA, which is consistent with findings of Einbu et al (Einbu et al 2013). The concentrations of NDELA and NHEGly (μmol/L) as function of time (days) for experiment A2-III (55 °C -21% O2 run 3), B2-II (65 °C -21% O2 run 2) and B4 (65 °C -98% O2) are shown in Figure 21.…”

Section: Nitrosaminessupporting

confidence: 92%

“…For degraded MEA N-nitrosodiethanolamine (NDELA), N-nitrosomorpholine (NMOR) and Nitrosodimethylamine (NDMA) were observed in both pilot samples and in samples from lab experiments (Fostås et al 2011;da Silva et al 2012). Formation of nitroso-(2-hydroxyethyl)-glycine (NHEGly) was also observed (Einbu et al 2013). NHEGly was a major contributor to the total nitrosamines observed in MEA samples from a tailored solvent degradation rig (SDR) (Einbu et al 2013), while NDELA was only observed in small amounts.…”

Section: Nitrosaminesmentioning

confidence: 98%

“…Formation of nitroso-(2-hydroxyethyl)-glycine (NHEGly) was also observed (Einbu et al 2013). NHEGly was a major contributor to the total nitrosamines observed in MEA samples from a tailored solvent degradation rig (SDR) (Einbu et al 2013), while NDELA was only observed in small amounts. The experiments presented in this work were conducted in campaigns spread over several years during which significant improvement in analytical techniques took place.…”

Section: Nitrosaminesmentioning

confidence: 98%

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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: Nitrosaminessupporting

confidence: 92%

Section: Nitrosaminesmentioning

confidence: 98%

Section: Nitrosaminesmentioning

confidence: 98%

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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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“…This indicates that unknown nitrosamines were present. This agrees with Einbu et al (2012) who reported that only few percent of nitrosamines present during their tests were found to be NDELA.…”

Section: Solvent Degradation During 30 Wt% Mea Campaignsupporting

confidence: 91%

Formation and Destruction of NDELA in 30 wt% MEA (Monoethanolamine) and 50 wt% DEA (Diethanolamine) Solutions

Knuutila

Asif

Vevelstad

et al. 2013

Oil Gas Sci. Technol. – Rev. IFP Energies nouvelles

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La destruction par irradiation UV de la NDELA pre´sente dans le solvant a aussi e´te´e´tudie´e sur la meˆme installation pilote. Deux campagnes de mesure ont e´te´mene´es, la premie`re utilisant une solution de 30 %m de monoe´thanolamine (MEA) et la seconde utilisant une solution de 50 %m de die´thanolamine (DEA). Durant la campagne de mesure sur la DEA, la destruction de la NDELA dans les eaux de nettoyage a aussi e´te´teste´e. De plus, la de´gradation thermique d'e´chantillons de solution de´grade´e pre´leve´s dans l'installation pilote a e´te´teste´e. Les re´sultats indiquent que de la NDELA se forme en pre´sence d'oxyde d'azote et de dioxyde d'azote. Il a e´te´constate´que la destruction de la NDELA par la lumie`re UV dans la boucle de solvant e´tait lente. La destruction de la NDELA par la lumie`re UV dans le compartiment des eaux de nettoyage a e´te´de´montre´e. La de´gradation de la NDELA durant des e´tudes de de´gradation thermique a`135°C a e´te´e´tablie.Abstract -Formation and Destruction of NDELA in 30 wt% MEA (Monoethanolamine) and 50 wt% DEA (Diethanolamine) Solutions -The formation of nitrosodiethanolamine (NDELA) in a lab scale pilot was studied by feeding known amounts of nitrogen oxide and nitrogen dioxide into the gas entering the absorber. In the same pilot, the destruction by UV-irradiation of NDELA present in the solvent was studied. Two campaigns were performed, one with 30 wt% monoethanolamine (MEA) and one with 50 wt% diethanolamine (DEA). During the DEA campaign the destruction of NDELA in the water wash section was also tested. Additionally, degraded solution samples withdrawn from the pilot were tested for thermal degradation. The results show that NDELA was formed when nitrogen oxide and nitrogen dioxide were present. Destruction of NDELA with UV-light in the solvent loop was found to be slow. In the water wash section, the UV-light destroyed the NDELA effectively. NDELA was found to degrade during the thermal degradation studies at 135°C.

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“…rich amine compared to lean amine (dilution of nitrosamine) and uncertainty of the method are 405 taken into account. These concentrations are quite high comparing to other results in the literature 406 (Einbu, 2013) and that could be due to the IFPEN pilot specifically. However, NDMA is known to be 407 carcinogenic and volatile.…”

supporting

confidence: 43%

Comprehensive monitoring of MEA degradation in a post-combustion CO2 capture pilot plant with identification of novel degradation products in gaseous effluents

Chahen

Huard

Cuccia

et al. 2016

International Journal of Greenhouse Gas Control

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24A pilot plant campaign was performed to study MEA degradation in CO 2 capture conditions and 25anticipate potential degradation products emissions to the atmosphere in industrial case. Aqueous 26 30% wt MEA was cycled between absorption and regeneration steps during 1700 hours in the 27 presence of a synthetic flue gas containing 81% of N 2 , 14% of CO 2 , 5% of O 2 , 97 ppm of NO, 9 ppm of 28 SO 2 and 5 ppm of NO 2 . Specific methods (sampling, sample conditioning and analysis) were 29 developed to improve degradation products identification and to provide a quantification of targeted 30 compounds in liquid phase and above all in absorber and stripper gas effluents. Especially, trace 31 elements were detected in liquid phase thanks to Head Space-Solid Phase MicroExtraction (HS-SPME) 32and liquid-liquid extraction with ChemElut cartridges and in gas phase thanks to adsorbent tubes of 33 different type: Sep-Pak  for aldehydes and ketones, Orbo 60 for N-nitrosodimethylamine, Tenax and 34 active charcoal for non-specific adsorption. 32 degradation products were identified in liquid phase 35 and 38 in gas phase, 17 of which for the first time, especially derivatives of pyridine and oxazolidine, 361H-pyrrole and a new nitrosamine, the N-nitroso-2-methyl-oxazolidine. 37 Keywords 38Ethanolamine degradation products in gas effluents; pilot plant monitoring; novel analytical 39 methods; solid phase extraction; nitrosamines; stripper gas effluents analysis. 40

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A new test rig for studies of degradation of CO2 absorption solvents at process conditions; comparison of test rig results and pilot plant data for degradation of MEA

Cited by 31 publications

References 3 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%

Formation and Destruction of NDELA in 30 wt% MEA (Monoethanolamine) and 50 wt% DEA (Diethanolamine) Solutions

Comprehensive monitoring of MEA degradation in a post-combustion CO2 capture pilot plant with identification of novel degradation products in gaseous effluents

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