Evaluation of a New Chemical Mechanism for 2‑Amino-2-methyl-1-propanol in a Reactive Environment from CSIRO Smog Chamber Experiments

• Published in: Environmental science & technology Vol. 54; no. 16; pp. 9844 - 9853
• Main Authors: Li, Kangwei, White, Stephen, Zhao, Bin, Geng, Chunmei, Halliburton, Brendan, Wang, Zhibin, Zhao, Yanyun, Yu, Hai, Yang, Wen, Bai, Zhipeng, Azzi, Merched
• Format: Journal Article
• Language: English
• Published: Easton American Chemical Society 18.08.2020; American Chemical Society (ACS)
• Subjects: Aerosols; Air pollution; Amines; Anthropogenic Impacts on the Atmosphere; Atmospheric chemistry; Atmospheric models; Carbon dioxide; Carbon sequestration; Chemical bonds; Chemical reactions; Chemical transport; Emissions; Flue gas; Gas streams; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Kinetic parameters; Kinetics; Nitrogen oxides; Organic compounds; Oxidation; Photochemistry; Photooxidation; Pollutants; Propanol; Reaction kinetics; Reactive environments; Smog; Smog chamber, AMP, Amine, CSIAMP-19, Chemical mechanism, Gas-phase chemistry; VOCs; Volatile organic compounds
• ISSN: 0013-936X; 1520-5851
• DOI: 10.1021/acs.est.9b07669

Amines are considered as an emerging class of atmospheric pollutants that are of great importance to atmospheric chemistry and new particle formation. As a typical amine, 2-amino-2-methyl-1-propanol (AMP) is one of the proposed solvents for capturing CO2 from flue gas streams in amine-based post-combustion CO2 capture plants, and it is expected to result in AMP emission and secondary product formation in the atmosphere. However, the current knowledge of its atmospheric chemistry and kinetics is poorly understood, particularly in a reactive environment. In this work, we used the CSIRO smog chamber to study the photo-oxidation of AMP in the presence of volatile organic compound (VOC)–NOx surrogate mixtures over a range of initial amine concentrations. O3 formation was significantly inhibited when AMP was added to the surrogate VOC–NOx mixtures, implying that AMP could alter known atmospheric chemical reaction pathways and the prevailing reactivity. Simultaneously, a large amount of AMP-derived secondary aerosol was formed, with a considerably high aerosol mass yield (i.e., ratio of aerosol formed to reacted AMP) of 1.06 ± 0.20. Based on updated knowledge of its kinetics, oxidation pathways, and product yields, we have developed a new mechanism (designated as CSIAMP-19), integrated it into the Carbon Bond 6 (CB6) chemical mechanism, and evaluated it against available smog chamber data. Compared with the existing AMP mechanism (designated as CarterAMP-08), the modified CB6 with CSIAMP-19 mechanism improves prediction against AMP–VOC–NOx experiments across a range of initial AMP concentrations, within ±10% model error for gross ozone production. Our results contribute to scientific understanding of AMP photochemistry and to the development of the chemical mechanism of other amines. Once some potential limitations are considered, the updated AMP reaction scheme can be further embedded into the chemical transport model for regional modeling scenarios where AMP-related emissions are of concern.