title: Effects of flue gas compositions on nitrosamine and nitramine formation in postcombustion CO2 capture systems.
abstract: Amine-based technologies are emerging as the prime contender for postcombustion CO2 capture. However, concerns have arisen over the health impacts of amine-based CO2 capture associated with the release of nitrosamines and nitramines, which are byproducts from the reactions between flue gas NOx and solvent amines. In this study, flue gas compositions were systematically varied to evaluate their effects on the formation of nitrosamines and nitramines in a lab-scale CO2 capture reactor with morpholine as a model solvent amine. The accumulation of N-nitrosomorpholine in both the absorber and washwater increased linearly with both NO and NO2 for concentrations up to ∼20 ppmv. These correlations could be extrapolated to estimate N-nitrosomorpholine accumulation at extremely low NOx levels (0.3 ppmv NO2 and 1.5 ppmv NO). NO played a particularly important role in driving N-nitrosomorpholine formation in the washwater, likely following partial oxidation to NO2 by O2. The accumulation of N-nitromorpholine in both the absorber and washwater positively correlated with flue gas NO2 concentration, but not with NO concentration. Both N-nitrosomorpholine and N-nitromorpholine accumulated fastest in the absence of CO2. Flue gas humidity did not affect nitrosamine accumulation in either the absorber or the washwater unit. These results provide a basis for estimating the effects of flue gas composition on nitrosamine and nitramine accumulation in postcombustion CO2 capture systems.
authors.affiliation: Department of Chemical and Environmental Engineering, Yale University , New Haven, Connecticut 06520, United States.
authors.forename: Ning
authors.initials: N
authors.lastname: Dai
authors.forename: William A
authors.initials: WA
authors.lastname: Mitch
mesh_terms: D000814:Aniline Compounds / Q000032:analysis / Q000138:chemical synthesis*; D002245:Carbon Dioxide / Q000737:chemistry* / Q000302:isolation & purification; D005740:Gases / Q000737:chemistry*; D009025:Morpholines / Q000032:analysis / Q000138:chemical synthesis / Q000737:chemistry; D009569:Nitric Oxide / Q000737:chemistry; D009573:Nitrites / Q000032:analysis; D009578:Nitrobenzenes / Q000032:analysis / Q000138:chemical synthesis*; D009585:Nitrogen Dioxide / Q000737:chemistry; D009602:Nitrosamines / Q000032:analysis / Q000138:chemical synthesis*; D010100:Oxygen / Q000737:chemistry; D012997:Solvents / Q000737:chemistry; D013997:Time Factors; D014867:Water / Q000737:chemistry
chemical_list: D000814:Aniline Compounds; D005740:Gases; D009025:Morpholines; D009573:Nitrites; D009578:Nitrobenzenes; D009602:Nitrosamines; D012997:Solvents; D014867:Water; D002245:Carbon Dioxide; D009569:Nitric Oxide; C002741:N-nitrosomorpholine; C031405:N-nitromorpholine; C037574:morpholine; C015384:nitramine; D009585:Nitrogen Dioxide; D010100:Oxygen