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Title: Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

Journal Article · · Atmospheric Environment (1994)
 [1];  [2];  [1];  [3];  [3];  [3];  [1]
  1. Beijing Key Lab. of Cloud, Beijing (China); Institute of Urban Meteorology, Beijing (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Beijing Key Lab. of Cloud, Beijing (China)

In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO2 and NOx, accelerated the formation of secondary inorganic aerosols, and led to rapid increase of the PM2.5 concentration.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
SC00112704
OSTI ID:
1228838
Alternate ID(s):
OSTI ID: 1250933
Report Number(s):
BNL-108476-2015-JA; R&D Project: 2015-BNL-EE631EECA-Budg; KP1703020
Journal Information:
Atmospheric Environment (1994), Vol. 122, Issue C; ISSN 1352-2310
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 100 works
Citation information provided by
Web of Science

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Cited By (10)

Persistent sulfate formation from London Fog to Chinese haze journal November 2016
Seasonal characteristics, formation mechanisms and source origins of PM2.5 in two megacities in Sichuan Basin, China journal January 2018
Vertical Characterization of Aerosol Particle Composition in Beijing, China: Insights From 3‐Month Measurements With Two Aerosol Mass Spectrometers journal November 2018
New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events journal April 2018
Relative humidity and O3 concentration as two prerequisites for sulfate formation journal January 2019
Primary and secondary aerosols in Beijing in winter: sources, variations and processes journal March 2016
Intermittent turbulence contributes to vertical dispersion of PM2.5 in the North China Plain: cases from Tianjin journal January 2018
Vertically resolved characteristics of air pollution during two severe winter haze episodes in urban Beijing, China journal January 2018
Primary and secondary aerosols in Beijing in winter: sources, variations and processes journal January 2016
Interactions between aerosol organic components and liquid water content during haze episodes in Beijing journal January 2019