Department of Chemical and Environmental Engineering, Yale University , New Haven, Connecticut 06520, United States.
Environ Sci Technol. 2014 Jul 1;48(13):7519-26. doi: 10.1021/es501864a. Epub 2014 Jun 19.
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.
胺基技术作为后燃烧 CO2 捕获的主要竞争者正在出现。然而,人们对与烟道气 NOx 和溶剂胺之间的反应产生的亚硝胺和硝胺有关的胺基 CO2 捕获的健康影响表示担忧。在这项研究中,系统地改变烟道气成分,以评估它们对以吗啉为模型溶剂胺的实验室规模 CO2 捕获反应器中亚硝胺和硝胺形成的影响。吸收器和洗涤水中 N-亚硝吗啉的积累与 NO 和 NO2 的浓度呈线性增加,最高可达约 20ppm。这些相关性可以外推以估计在极低的 NOx 水平(0.3ppm 二氧化氮和 1.5ppm 一氧化氮)下 N-亚硝吗啉的积累。NO 在推动洗涤水中 N-亚硝吗啉的形成方面发挥了特别重要的作用,可能是通过 O2 部分氧化为 NO2。吸收器和洗涤水中 N-硝吗啉的积累与烟道气 NO2 浓度呈正相关,但与 NO 浓度无关。在没有 CO2 的情况下,N-亚硝吗啉和 N-硝吗啉积累最快。烟道气湿度对吸收器和洗涤器单元中亚硝胺的积累没有影响。这些结果为估计烟道气成分对后燃烧 CO2 捕获系统中亚硝胺和硝胺积累的影响提供了依据。