An unexpected large continental source of reactive bromine and chlorine with significant impact on wintertime air quality

Peng, Xiang; Wang, Weihao; Xia, Men; Chen, Hui; Ravishankara, A. R.; Li, Qinyi; Saiz‐Lopez, Alfonso; Liu, Pengfei; Zhang, Fei; Zhang, Chenglong; Xue, Likun; Wang, Xinfeng; George, Christian; Wang, Jinhe; Mu, Yujing; Chen, Jianmin; Wang, Tao

doi:10.1002/essoar.10504290.1

Cited by 11 publications

(20 citation statements)

References 22 publications

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“…Bromine showed a good correlation with CCOA ( r 2 = 0.49, Figure 10a), indicating coal combustion emission was a significant source of bromine. This result is consistent with previous studies (Peng et al., 2020; Smyth et al., 2013) that industrial or combustion‐related sources and coal‐burning were major sources of both reactive gases and particle bromine. The diurnal cycle of bromine presented higher concentration at nighttime and exhibited a pronounced morning peak, which is similar to that of CCOA.…”

Section: Resultssupporting

confidence: 93%

“…Reactive halogen species play an important role in atmospheric chemistry and affect the ozone formation substantially. Previous studies at the rural site in NCP have found unexpectedly high concentration of reactive bromine and chlorine, particularly BrCl in rural area in NCP, which was mainly from residential coal burning and photochemical process (Peng et al., 2020). In this study, we observed several particulate halide species, that is, iodine (I + ) and bromine (Br + ) that are well separated from high‐resolution mass spectra (Figure S2 in Supporting Information ).…”

Section: Resultsmentioning

confidence: 92%

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Primary Emissions and Secondary Aerosol Processing During Wintertime in Rural Area of North China Plain

Chen

Qiu

et al. 2022

JGR Atmospheres

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The vast rural areas often experience more severe haze pollution than megacities during wintertime in North China Plain (NCP), yet the sources and evolution processes of aerosol particles, particularly organic aerosol (OA) remain poorly understood. Here we conducted real‐time measurements of submicron aerosol (PM1) species using a high‐resolution aerosol mass spectrometer at a representative rural site in NCP in winter 2019. Our results showed the dominance of organics (36%) and nitrate in PM1 (22%) in 2019. Positive matrix factorization analysis illustrated similarly important primary sources from traffic emissions, coal combustion, and biomass burning, yet secondary OA (SOA) from photochemical and aqueous‐phase related processing exceeded primary OA (53% vs. 47%). Substantial decreases in primary species and considerable increases in nitrate and sulphate were observed since winter 2018, demonstrating enhanced secondary formation in winter 2019. OA composition changed significantly from clean period to fog events with the contribution of aqueous phase‐related oxygenated OA increasing from 6% to 44%, while the photochemical SOA decreased correspondingly from 51% to 19%. The size distributions of aerosol species also changed by shifting toward large sizes during fog events. Elemental analysis of OA and the Van Krevelen diagram (H/C vs. O/C) illustrated the different roles of photochemical and aqueous‐phase processing during daytime and nighttime, respectively, and aqueous‐phase processing is subject to the formation of organic compounds with high H/C and O/C ratios. The large differences in fog processing of submicron aerosol species between 2018 and 2019 due to different temperatures were also elucidated.

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Section: Resultssupporting

confidence: 93%

Section: Resultsmentioning

confidence: 92%

Primary Emissions and Secondary Aerosol Processing During Wintertime in Rural Area of North China Plain

Chen

Qiu

et al. 2022

JGR Atmospheres

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“…A tomic chlorine (Cl) is a very reactive radical, known to destroy stratospheric ozone (O 3 ) through catalytic cycles 1,2 . In the lower troposphere, it can initiate the oxidation of volatile organic compounds (VOCs), increase the levels of conventional radicals (OH, HO 2 and RO 2 ), and produce O 3 and secondary organic aerosols (SOA) [3][4][5][6][7] which are air pollutants and also alter the Earth's radiation budget and climate. Cl reacts rapidly with methane, the most abundant hydrocarbon and the secondmost important greenhouse gas emitted into the atmosphere 8,9 .…”

mentioning

confidence: 99%

“…Previously, Cl 2 has been measured in the lower troposphere in locations such as at the Arctic surface 11,12 , the marine boundary layer [13][14][15] , and continental sites 16,17 . Cl 2 was found to typically peak during nighttime, but elevated levels (17-450 pptv) have also been observed during daytime 6,11,12,[18][19][20][21] . The daytime occurrence of Cl 2 is of great importance as it may have a profound impact on atmospheric photochemistry and oxidation capacity 6,19 .…”

mentioning

confidence: 99%

“…Cl 2 was found to typically peak during nighttime, but elevated levels (17-450 pptv) have also been observed during daytime 6,11,12,[18][19][20][21] . The daytime occurrence of Cl 2 is of great importance as it may have a profound impact on atmospheric photochemistry and oxidation capacity 6,19 . Such observations also reveal the existence of a significant Cl 2 source that compensates or even overcomes its fast photolytic loss.…”

mentioning

confidence: 99%

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Photodissociation of particulate nitrate as a source of daytime tropospheric Cl2

Peng

Wang

et al. 2022

Preprint

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Chlorine atoms (Cl) are highly reactive and can strongly influence the abundances of climate and air quality-relevant trace gases. Despite extensive research on molecular chlorine (Cl 2 ), a Cl precursor, in the polar atmosphere, its sources in other regions are still poorly understood.Here we report the daytime Cl 2 concentrations of up to 1 ppbv observed in a coastal area of Hong Kong, revealing a large daytime source of Cl 2 (2.7 pptv s −1 at noon). Field and laboratory experiments indicate that photodissociation of particulate nitrate by sunlight under acidic conditions (pH < 3.0) can activate chloride and account for the observed daytime Cl 2 production. The high Cl 2 concentrations significantly increased atmospheric oxidation. Given the ubiquitous existence of chloride, nitrate, and acidic aerosols, we propose that nitrate photolysis is a significant daytime chlorine source globally. This so far unaccounted for source of chlorine can have substantial impacts on atmospheric chemistry.

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Assessment of trace elements directly from archived total suspended particulate filters by laser ablation ICP-MS: A case study of South Carolina

Commodore

Christopher

Wolf

et al. 2023

Journal of Trace Elements and Minerals

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An unexpected large continental source of reactive bromine and chlorine with significant impact on wintertime air quality

Cited by 11 publications

References 22 publications

Primary Emissions and Secondary Aerosol Processing During Wintertime in Rural Area of North China Plain

Primary Emissions and Secondary Aerosol Processing During Wintertime in Rural Area of North China Plain

Photodissociation of particulate nitrate as a source of daytime tropospheric Cl2

Assessment of trace elements directly from archived total suspended particulate filters by laser ablation ICP-MS: A case study of South Carolina

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