TY - JOUR
T1 - Heterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China
T2 - Roles of aerosol water content and chemical composition
AU - Jun Tham, Yee
AU - Wang, Zhe
AU - Li, Qinyi
AU - Wang, Weihao
AU - Wang, Xinfeng
AU - Lu, Keding
AU - Ma, Nan
AU - Yan, Chao
AU - Kecorius, Simonas
AU - Wiedensohler, Alfred
AU - Zhang, Yuanhang
AU - Wang, Tao
PY - 2018/9/12
Y1 - 2018/9/12
N2 - Heterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (3(N2O5)) and ClNO2 production yield (•) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined 3(N2O5) and • values varied greatly, with an average of 0.022 for 3(N2O5) (±0.012, standard deviation) and 0.34 for • (±0.28, standard deviation). The variations in 3(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived • showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for 3(N2O5) and • to accurately assess photochemical and haze pollution.
AB - Heterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (3(N2O5)) and ClNO2 production yield (•) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined 3(N2O5) and • values varied greatly, with an average of 0.022 for 3(N2O5) (±0.012, standard deviation) and 0.34 for • (±0.28, standard deviation). The variations in 3(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived • showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for 3(N2O5) and • to accurately assess photochemical and haze pollution.
UR - http://www.scopus.com/inward/record.url?scp=85053341788&partnerID=8YFLogxK
U2 - 10.5194/acp-18-13155-2018
DO - 10.5194/acp-18-13155-2018
M3 - Journal article
AN - SCOPUS:85053341788
SN - 1680-7316
VL - 18
SP - 13155
EP - 13171
JO - Atmospheric Chemistry and Physics
JF - Atmospheric Chemistry and Physics
IS - 17
ER -