Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines

Na Rae Choi; Seungshik Park; Seoryeong Ju; Yong Bin Lim; Ji Yi Lee; Eunhye Kim; Soontae Kim; Hye Jung Shin; Yong Pyo Kim

doi:10.1016/j.envpol.2022.119142

Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines

Na Rae Choi, Seungshik Park, Seoryeong Ju, Yong Bin Lim, Ji Yi Lee, Eunhye Kim, Soontae Kim, Hye Jung Shin, Yong Pyo Kim

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Abstract

Contribution of liquid water content (LWC) to the levels of the carcinogenic particulate nitro(so) compounds and the chemistry affecting LWC were investigated based on the observation of seven nitrosamines and two nitramines in rural (Seosan) and urban (Seoul) area in South Korea during October 2019 and a model simulation. The concentrations of both the total nitrosamines and nitramines were higher in Seosan (12.48 ± 16.12 ng/m³ and 0.65 ± 0.71 ng/m³, respectively) than Seoul (7.41 ± 13.59 ng/m³ and 0.24 ± 0.15 ng/m³, respectively). The estimated LWC using a thermodynamic model in Seosan (12.92 ± 9.77 μg/m³) was higher than that in Seoul (6.20 ± 5.35 μg/m³) mainly due to higher relative humidity (75 ± 9% (Seosan); 62 ± 10% (Seoul)) and higher concentrations of free ammonia (0.13 ± 0.09 μmol/m³ (Seosan); 0.08 ± 0.01 μmol/m³ (Seoul)) and total nitric acid (0.09 ± 0.07 μmol/m³ (Seosan); 0.04 ± 0.02 μmol/m³ (Seoul)) in Seosan while neither fog nor rain occurred during the sampling period. The relatively high concentrations of the particulate nitrosamines (>30 ng/m³) only observed probably due to the higher LWC (>10 μg/m³) in Seosan. It implies that aqueous phase reactions involving NO₂ and/or uptake from the gas phase enhanced by LWC could be promoted in Seosan. Strong correlation between the concentrations of nitrosodi-methylamine (NDMA), an example of nitrosamines, simulated by a kinetic box model including the aqueous phase reactions and the measured concentration of NDMA in Seosan (R = 0.77; 0.37 (Seoul)) indicates that the aqueous phase reactions dominantly enhanced the NDMA concentrations in Seosan. On the other hand, it is estimated that the formation of nitrosamines by aqueous phase reaction was not significant due to the relatively lower LWC in Seoul compared to that in Seosan. Furthermore, it is presumed that nitramines are mostly emitted from the primary emission sources. This study implies that the concentration of the particulate nitrosamines can be promoted by aqueous phase reaction enhanced by LWC.

Original language	English
Article number	119142
Journal	Environmental Pollution
Volume	303
DOIs	https://doi.org/10.1016/j.envpol.2022.119142
State	Published - 15 Jun 2022

Bibliographical note

Funding Information:
This work was supported by the Technology Development Program to Solve Climate Changes ( NRF-2019M1A2A2103953 ) and Basic Science Research Program ( NRF-2020R1F1A1050361 ) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, Information & Communication Technology (ICT). N. R. Choi is grateful for the Solvay Scholarship and the Ministry of Education ( NRF-2021R1A6A3A03039361 ). Y. B. Lim acknowledge the support from Fine Particle Research Initiative in East Asia Considering National Differences (FRIEND) Project through NRF funded by Ministry of Science and ICT ( NRF-2020M3G1A1114537 ) and Basic Science Research Program through NRF funded by Ministry of Education ( NRF-2021R1I1A1A01059748 ) in South Korea. This work was also supported, in part, by the Korea National Institute of Environmental Research ( NIER-2021-03-03-001 ).

Publisher Copyright:
© 2022

Keywords

Atmospheric reaction
Free ammonia
Liquid water content
Nitramines
Nitrosamines
Seosan
Seoul

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10.1016/j.envpol.2022.119142

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title = "Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines",

abstract = "Contribution of liquid water content (LWC) to the levels of the carcinogenic particulate nitro(so) compounds and the chemistry affecting LWC were investigated based on the observation of seven nitrosamines and two nitramines in rural (Seosan) and urban (Seoul) area in South Korea during October 2019 and a model simulation. The concentrations of both the total nitrosamines and nitramines were higher in Seosan (12.48 ± 16.12 ng/m3 and 0.65 ± 0.71 ng/m3, respectively) than Seoul (7.41 ± 13.59 ng/m3 and 0.24 ± 0.15 ng/m3, respectively). The estimated LWC using a thermodynamic model in Seosan (12.92 ± 9.77 μg/m3) was higher than that in Seoul (6.20 ± 5.35 μg/m3) mainly due to higher relative humidity (75 ± 9% (Seosan); 62 ± 10% (Seoul)) and higher concentrations of free ammonia (0.13 ± 0.09 μmol/m3 (Seosan); 0.08 ± 0.01 μmol/m3 (Seoul)) and total nitric acid (0.09 ± 0.07 μmol/m3 (Seosan); 0.04 ± 0.02 μmol/m3 (Seoul)) in Seosan while neither fog nor rain occurred during the sampling period. The relatively high concentrations of the particulate nitrosamines (>30 ng/m3) only observed probably due to the higher LWC (>10 μg/m3) in Seosan. It implies that aqueous phase reactions involving NO2 and/or uptake from the gas phase enhanced by LWC could be promoted in Seosan. Strong correlation between the concentrations of nitrosodi-methylamine (NDMA), an example of nitrosamines, simulated by a kinetic box model including the aqueous phase reactions and the measured concentration of NDMA in Seosan (R = 0.77; 0.37 (Seoul)) indicates that the aqueous phase reactions dominantly enhanced the NDMA concentrations in Seosan. On the other hand, it is estimated that the formation of nitrosamines by aqueous phase reaction was not significant due to the relatively lower LWC in Seoul compared to that in Seosan. Furthermore, it is presumed that nitramines are mostly emitted from the primary emission sources. This study implies that the concentration of the particulate nitrosamines can be promoted by aqueous phase reaction enhanced by LWC.",

keywords = "Atmospheric reaction, Free ammonia, Liquid water content, Nitramines, Nitrosamines, Seosan, Seoul",

author = "Choi, {Na Rae} and Seungshik Park and Seoryeong Ju and Lim, {Yong Bin} and Lee, {Ji Yi} and Eunhye Kim and Soontae Kim and Shin, {Hye Jung} and Kim, {Yong Pyo}",

note = "Funding Information: This work was supported by the Technology Development Program to Solve Climate Changes ( NRF-2019M1A2A2103953 ) and Basic Science Research Program ( NRF-2020R1F1A1050361 ) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, Information & Communication Technology (ICT). N. R. Choi is grateful for the Solvay Scholarship and the Ministry of Education ( NRF-2021R1A6A3A03039361 ). Y. B. Lim acknowledge the support from Fine Particle Research Initiative in East Asia Considering National Differences (FRIEND) Project through NRF funded by Ministry of Science and ICT ( NRF-2020M3G1A1114537 ) and Basic Science Research Program through NRF funded by Ministry of Education ( NRF-2021R1I1A1A01059748 ) in South Korea. This work was also supported, in part, by the Korea National Institute of Environmental Research ( NIER-2021-03-03-001 ). Publisher Copyright: {\textcopyright} 2022",

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day = "15",

doi = "10.1016/j.envpol.2022.119142",

language = "English",

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T1 - Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines

AU - Choi, Na Rae

AU - Park, Seungshik

AU - Ju, Seoryeong

AU - Lim, Yong Bin

AU - Lee, Ji Yi

AU - Kim, Eunhye

AU - Kim, Soontae

AU - Shin, Hye Jung

AU - Kim, Yong Pyo

N1 - Funding Information: This work was supported by the Technology Development Program to Solve Climate Changes ( NRF-2019M1A2A2103953 ) and Basic Science Research Program ( NRF-2020R1F1A1050361 ) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, Information & Communication Technology (ICT). N. R. Choi is grateful for the Solvay Scholarship and the Ministry of Education ( NRF-2021R1A6A3A03039361 ). Y. B. Lim acknowledge the support from Fine Particle Research Initiative in East Asia Considering National Differences (FRIEND) Project through NRF funded by Ministry of Science and ICT ( NRF-2020M3G1A1114537 ) and Basic Science Research Program through NRF funded by Ministry of Education ( NRF-2021R1I1A1A01059748 ) in South Korea. This work was also supported, in part, by the Korea National Institute of Environmental Research ( NIER-2021-03-03-001 ). Publisher Copyright: © 2022

PY - 2022/6/15

Y1 - 2022/6/15

N2 - Contribution of liquid water content (LWC) to the levels of the carcinogenic particulate nitro(so) compounds and the chemistry affecting LWC were investigated based on the observation of seven nitrosamines and two nitramines in rural (Seosan) and urban (Seoul) area in South Korea during October 2019 and a model simulation. The concentrations of both the total nitrosamines and nitramines were higher in Seosan (12.48 ± 16.12 ng/m3 and 0.65 ± 0.71 ng/m3, respectively) than Seoul (7.41 ± 13.59 ng/m3 and 0.24 ± 0.15 ng/m3, respectively). The estimated LWC using a thermodynamic model in Seosan (12.92 ± 9.77 μg/m3) was higher than that in Seoul (6.20 ± 5.35 μg/m3) mainly due to higher relative humidity (75 ± 9% (Seosan); 62 ± 10% (Seoul)) and higher concentrations of free ammonia (0.13 ± 0.09 μmol/m3 (Seosan); 0.08 ± 0.01 μmol/m3 (Seoul)) and total nitric acid (0.09 ± 0.07 μmol/m3 (Seosan); 0.04 ± 0.02 μmol/m3 (Seoul)) in Seosan while neither fog nor rain occurred during the sampling period. The relatively high concentrations of the particulate nitrosamines (>30 ng/m3) only observed probably due to the higher LWC (>10 μg/m3) in Seosan. It implies that aqueous phase reactions involving NO2 and/or uptake from the gas phase enhanced by LWC could be promoted in Seosan. Strong correlation between the concentrations of nitrosodi-methylamine (NDMA), an example of nitrosamines, simulated by a kinetic box model including the aqueous phase reactions and the measured concentration of NDMA in Seosan (R = 0.77; 0.37 (Seoul)) indicates that the aqueous phase reactions dominantly enhanced the NDMA concentrations in Seosan. On the other hand, it is estimated that the formation of nitrosamines by aqueous phase reaction was not significant due to the relatively lower LWC in Seoul compared to that in Seosan. Furthermore, it is presumed that nitramines are mostly emitted from the primary emission sources. This study implies that the concentration of the particulate nitrosamines can be promoted by aqueous phase reaction enhanced by LWC.

AB - Contribution of liquid water content (LWC) to the levels of the carcinogenic particulate nitro(so) compounds and the chemistry affecting LWC were investigated based on the observation of seven nitrosamines and two nitramines in rural (Seosan) and urban (Seoul) area in South Korea during October 2019 and a model simulation. The concentrations of both the total nitrosamines and nitramines were higher in Seosan (12.48 ± 16.12 ng/m3 and 0.65 ± 0.71 ng/m3, respectively) than Seoul (7.41 ± 13.59 ng/m3 and 0.24 ± 0.15 ng/m3, respectively). The estimated LWC using a thermodynamic model in Seosan (12.92 ± 9.77 μg/m3) was higher than that in Seoul (6.20 ± 5.35 μg/m3) mainly due to higher relative humidity (75 ± 9% (Seosan); 62 ± 10% (Seoul)) and higher concentrations of free ammonia (0.13 ± 0.09 μmol/m3 (Seosan); 0.08 ± 0.01 μmol/m3 (Seoul)) and total nitric acid (0.09 ± 0.07 μmol/m3 (Seosan); 0.04 ± 0.02 μmol/m3 (Seoul)) in Seosan while neither fog nor rain occurred during the sampling period. The relatively high concentrations of the particulate nitrosamines (>30 ng/m3) only observed probably due to the higher LWC (>10 μg/m3) in Seosan. It implies that aqueous phase reactions involving NO2 and/or uptake from the gas phase enhanced by LWC could be promoted in Seosan. Strong correlation between the concentrations of nitrosodi-methylamine (NDMA), an example of nitrosamines, simulated by a kinetic box model including the aqueous phase reactions and the measured concentration of NDMA in Seosan (R = 0.77; 0.37 (Seoul)) indicates that the aqueous phase reactions dominantly enhanced the NDMA concentrations in Seosan. On the other hand, it is estimated that the formation of nitrosamines by aqueous phase reaction was not significant due to the relatively lower LWC in Seoul compared to that in Seosan. Furthermore, it is presumed that nitramines are mostly emitted from the primary emission sources. This study implies that the concentration of the particulate nitrosamines can be promoted by aqueous phase reaction enhanced by LWC.

KW - Atmospheric reaction

KW - Free ammonia

KW - Liquid water content

KW - Nitramines

KW - Nitrosamines

KW - Seosan

KW - Seoul

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DO - 10.1016/j.envpol.2022.119142

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VL - 303

JO - Environmental Pollution

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Contribution of liquid water content enhancing aqueous phase reaction forming ambient particulate nitrosamines

Abstract

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Keywords

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