Gas-Phase Reactions of (CH3)2N Radicals with NO and NO2

Lazarou, Yannis G.; Kambanis, Kyriakos G.; Papagiannakopoulos, Panos

doi:10.1021/j100059a022

Cited by 27 publications

(19 citation statements)

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“…Normalizing to k 3 , the branching ratios in the amino radical reactions with O 2 , NO and NO 2 are therefore k 2 /k 3 = 0.264 AE 0.023, k 5 /k 3 = (3.90 AE 0.28) Â 10 À7 and k 4 /k 3 = 0.22 AE 0.06. Lazarou et al 51 studied the reactions of the (CH 3 ) 2 N radical with NO and NO 2 by the Very Low Pressure Reactor (VLPR) technique and reported absolute rates of reaction k 2 = (8.53 AE 1.42) Â 10 À14 and k 3 = (3.18 AE 0.48) Â 10 À13 cm 3 molecule À1 s À1 at 300 K. In addition, they reported k = (6.36 AE 0.74) Â 10 À13 cm 3 molecule À1 s À1 at 300 K for a competing NO 2 reaction:…”

Section: Nitrosamine and Nitramine Formationmentioning

confidence: 99%

Atmospheric chemistry and environmental impact of the use of amines in carbon capture and storage (CCS)

2012

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This critical review addresses the atmospheric gas phase and aqueous phase amine chemistry that is relevant to potential emissions from amine-based carbon capture and storage (CCS). The focus is on amine, nitrosamine and nitramine degradation, and nitrosamine and nitramine formation processes. A comparison between the relative importance of the various atmospheric sinks for amines, nitrosamines and nitramines is presented.

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Section: Nitrosamine and Nitramine Formationmentioning

confidence: 99%

Atmospheric chemistry and environmental impact of the use of amines in carbon capture and storage (CCS)

2012

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“…for which experimental results of 0.63 : 0.37 12 and 0.58 : 0.42, 8 and a theoretical result of 0.52 : 0.48 9 are available for the CH : NH branching ratio. Smog chamber and laboratory studies of dimethylamine and the dimethylamino radical, 6,8,[11][12][13][14][15] of trimethylamine, 4,8 and of diethylamine and triethylamine, 4,15 have established that amino radicals react with O 2 , NO 2 and NO -in the latter case leading to the formation of an N-nitroso amine (nitrosamine). Recent results from smog chamber photo-oxidation studies of methylamine 8 and ethylamine 15 show the formation of N-nitro methylamine (methylnitramine) and N-nitro ethylamine (ethylnitramine), whereas N-nitroso methylamine (methylnitrosamine) and N-nitroso ethylamine were not detected.…”

Section: Introductionmentioning

confidence: 99%

Do primary nitrosamines form and exist in the gas phase? A computational study of CH3NHNO and (CH3)2NNO

Tang

Hanrath

Nielsen

2012

Phys. Chem. Chem. Phys.

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The reactions of the CH(3)NH and (CH(3))(2)N radicals with NO have been studied using quantum chemistry methods to compare the formation and stability of primary and secondary nitrosamines. The calculations show that the entrance part of potential energy surfaces of CH(3)NHNO and (CH(3))(2)NNO formation are similar, and it is concluded that primary amines form nitrosamines under the atmospheric conditions. CH(3)NHNO can, in contrast to (CH(3))(2)NNO, undergo isomerization via a barrier below the reactants entrance energy to CH(2)NHNOH, which through reaction with O(2) eventually leads to formation of CH(2)=NH on a short timescale. TDDFT, CASPT2 and MR-CI calculations show little difference between the n→π* transitions in CH(3)NHNO and (CH(3))(2)NNO and that the two molecules should have comparable photolysis lifetimes in the atmosphere.

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“…MEA-Simple uses rate constant k 3a = 3.20 × x10 − 13 cm 3 molecule − 1 s − 1 as determined by Lazarou et al (1994) for the reaction of the dimethyl amino radical with NO 2 . MEA-Detail uses rate constant k 3a = 7.0 × x10 − 14 cm 3 molecule − 1 s − 1 as reported by Nielsen et al (2010).…”

Section: Elsevier_stoten_17722mentioning

confidence: 99%

“…The rate k 3a ·[NO 2 ] for the reaction of the N-amino radical to give MEA-nitramine in the scheme MEA-Detail (Karl et al, 2012) was found to be four times smaller than in the scheme MEA-Simple. MEA-Simple, which has been applied in the WRF--EMEP model framework, uses rate constant k 3a with a value determined by Lazarou et al (1994) for the reaction of the dimethyl amino radical with NO 2 . MEA-Detail on the other hand, which uses k 3a as reported by Nielsen et al (2010), has been evaluated in EUPHORE chamber experiments (Karl et al, 2012).…”

Section: Model Comparison and Sensitivity Analysismentioning

confidence: 99%

Modelling atmospheric oxidation of 2-aminoethanol (MEA) emitted from post-combustion capture using WRF–Chem

Karl

Svendby

Walker

et al. 2015

Science of The Total Environment

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Limiting global warming to less than 2 °C relative to pre-industrial levels would require substantial cuts in anthropogenic emissions of greenhouse gases (IPCC, 2014). Carbon capture and storage (CCS) is an important mitigation technology for reducing anthropogenic carbon dioxide (CO 2 ) emissions from industrial and energy-related point sources. In this process, CO 2 is captured, conditioned, compressed and transported to a storage location for long-term isolation from the atmosphere. Several problems can occur during CCS with impacts on the environment. Post-combustion capture from power plants entails emissions of pollutants, solvents and its degradation by-products to the atmosphere, emissions to water and generation of solid waste (e.g. Reynolds et al., 2012). During the further steps of the CCS chain, CO 2 release during transport in pipelines as well as the escape of injected CO 2 from the storage location to the atmosphere or groundwater pose risks to the environment (Koorneef et al., 2012).Modelling atmospheric oxidation of 2-aminoethanol (MEA) emitted from post-combustion capture using WRF--Chem AbstractCarbon capture and storage (CCS) is a technological solution that can reduce the amount of carbon dioxide (CO 2 ) emissions from the use of fossil fuel in power plants and other industries. A leading method today is amine based post-combustion capture, in which 2-aminoethanol (MEA) is one of the most studied absorption solvents. In this process, amines are released to the atmosphere through evaporation and entrainment from the CO 2 absorber column. Modelling is a key instrument for simulating the atmospheric dispersion and chemical transformation of MEA, and for projections of ground-level air concentrations and deposition rates. In this study, the Weather Research and Forecasting model inline coupled with chemistry, WRF--Chem, was applied to quantify the impact of using a comprehensive MEA photo-oxidation sequence compared to using a simplified MEA scheme. Main discrepancies were found for iminoethanol (roughly doubled in the detailed scheme) and 2-nitro aminoethanol, short MEA-nitramine (reduced by factor of two in the detailed scheme). The study indicates that MEA emissions from a full-scale capture plant can modify regional background levels of isocyanic acid. Predicted atmospheric concentrations of isocyanic acid were however below the limit value of 1 ppbv for ambient exposure. The dependence of the formation of hazardous compounds in the OH-initiated oxidation of MEA on ambient levels level of nitrogen oxides (NO x ) was studied in a scenario without NO x emissions from a refinery area in the vicinity of the capture plant. Hourly MEAnitramine peak concentrations higher than 40 pg m − 3 did only occur when NO x mixing ratios were above 2 ppbv. Therefore, the spatial variability and temporal variability of levels of OH and NO x need to be taken into account in the health risk assessment. The health risk due to direct emissions of nitrosamines and nitramines from full-scale CO 2 capture should be i...

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Gas-Phase Reactions of (CH3)2N Radicals with NO and NO2

Cited by 27 publications

References 4 publications

Atmospheric chemistry and environmental impact of the use of amines in carbon capture and storage (CCS)

Atmospheric chemistry and environmental impact of the use of amines in carbon capture and storage (CCS)

Do primary nitrosamines form and exist in the gas phase? A computational study of CH3NHNO and (CH3)2NNO

Modelling atmospheric oxidation of 2-aminoethanol (MEA) emitted from post-combustion capture using WRF–Chem

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