Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes

Lin, Mang; Biglari, Saman; Zhang, Zhi Sheng; Crocker, Daniel R.; Tao, Jun; Su, Binbin; Liu, Lanzhong; Thiemens, M. H.

doi:10.1002/2017gl073637

Cited by 24 publications

(19 citation statements)

References 64 publications

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“…Alternatively, the discrepancy may be due to our use of aerosol [Na + ] to estimate SO 4 2− SS rather than [Mg 2+ ] used by Sievering et al (). Sodium is the most widely used conservative tracer of sea salt (Lin et al, ; Norman et al, ; Udisti et al, ) because (1) it has a high concentration in the seawater, (2) nonmarine sodium inputs are trivial in most places (McInnes et al, ), and (3) it is insensitive to secondary alterations. Sievering et al () used [Mg 2+ ] to calculate SO 4 2− SS fraction because of abnormally high [Na + Cl − ] and [Na + Mg 2+ ] ratios in their aerosols that they attributed to either contamination by filter blanks or possible contributions of sodium in soil.…”

Section: Resultsmentioning

confidence: 99%

“…Alternatively, the discrepancy may be due to our use of aerosol [Na + ] to estimate SO 4 2À SS rather than [Mg 2+ ] used by Sievering et al (2004). Sodium is the most widely used conservative tracer of sea salt (Lin et al, 2017;Norman et al, 1999;Udisti et al, 2016) because (1) it has a high concentration in the seawater, (2)…”

Section: Distribution Of Sea-salt and Nonsea-salt Sulfate In Coarse Amentioning

confidence: 99%

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Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

Michalski

Davy

et al. 2018

Geophysical Research Letters

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Marine sulfate aerosols in the Southern Ocean are critical to the global radiation balance, yet the sources of sulfate and their seasonal variations are unclear. We separately sampled marine and ambient aerosols at Baring Head, New Zealand for 1 year using two collectors and evaluated the sources of sulfate in coarse (1–10 μm) and fine (0.05–1 μm) aerosols using sulfur isotopes (δ34S). In both collectors, sea‐salt sulfate (SO42−SS) mainly existed in coarse aerosols and nonsea‐salt sulfate (SO42−NSS) dominated the sulfate in fine aerosols, although some summer SO42−NSS appeared in coarse particles due to aerosol coagulation. SO42−NSS in the marine aerosols was mainly (88–100%) from marine biogenic dimethylsulfide (DMS) emission, while the SO42−NSS in the ambient aerosols was a combination of DMS (73–79%) and SO2 emissions from shipping activities (~21–27%). The seasonal variations of SO42−NSS concentrations inferred from the δ34S values in both collectors were mainly controlled by the DMS flux.

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Section: Resultsmentioning

confidence: 99%

Section: Distribution Of Sea-salt and Nonsea-salt Sulfate In Coarse Amentioning

confidence: 99%

Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

Michalski

Davy

et al. 2018

Geophysical Research Letters

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“…It is worth to note that several recent studies have highlighted the important role NO 2 might play in sulfate formation in the polluted environment in China (Cheng et al, 2016;Wang et al, 2016a;Xie et al, 2015a). Nevertheless, the aqueous SO 2 + H 2 O 2 /O 3 oxidation should still be the dominant mechanism in most cases, especially at a background site (Lin et al, 2017). The aqueous SO 2 + oxygen (catalyzed by Fe (III)) reaction can also be important under heavy haze conditions in north China .…”

Section: Interannual Variations In Beijingmentioning

confidence: 99%

A review of current knowledge concerning PM<sub>2. 5</sub> chemical composition, aerosol optical properties and their relationships across China

et al. 2017

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Abstract. To obtain a thorough knowledge of PM 2.5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM 2.5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM 2.5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM 2.5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO 2− 4 ) and ammonium (NH + 4 ) remained at high levels, and nitrate (NO − 3 ) increased. The highest seasonal averages of PM 2.5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM 2.5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM 2.5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM 2.5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM 2.5 mass in applicable cities.The geographical pattern of scattering coefficient (b sp ) was similar to that of PM 2.5 , and that of aerosol absorption coefficient (b ap ) was determined by elemental carbon (EC) mass concentration and its coating. b sp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions. Secondary inorganic aerosols accounted for about 60 % of aerosol extinction coefficient (b ext ) at RH greater than 70 %. The mass scattering efficiency (MSE) of PM 2.5 ranged from 3.0 to 5.0 m 2 g −1 for aerosols produced from anthropogenic emissions and from 0.7 to 1.0 m 2 g −1 for natural dust aerosols. The mass absorption efficiency (MAE) of EC ranged from 6.5 to 12.4 m 2 g −1 in urban environments, but the MAE of water-soluble organic carbon was only 0.05 to 0.11 m 2 g −1 . Historical emission control policies in China and their effectiveness were discussed based on available chemically resolved PM 2.5 data, which provides the much needed knowledge for guiding future studies and emissions policies.

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“…1b) (Lin et al, 2017;Li et al, 2013) and other midlatitude sites (Table S6). The overall 17 O obs levels during our entire sampling time are similar for NPDs and PDs, being (0.9 ± 0.1) and (0.9 ± 0.4) ‰, respectively.…”

Section: Characteristics Of Haze Events In Beijingmentioning

confidence: 99%

Isotopic constraints on heterogeneous sulfate production in Beijing haze

et al. 2018

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Abstract. Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter) in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM 2.5 sulfate ( 17 O(SO 2− 4 )) collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 12-hourly averaged PM 2.5 concentrations ranged from 16 to 323 µg m −3 with a mean of (141 ± 88 (1σ )) µg m −3 , with SO Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM 2.5 ≥ 75 µg m −3 ) of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68 %. During PDs of Cases I and III-V, heterogeneous sulfate production (P het ) was estimated to contribute 41-54 % to total sulfate formation with a mean of (48 ± 5) %. For the specific mechanisms of heterogeneous oxidation of SO 2 , chemical reaction kinetics calculations suggested S(IV) (= SO 2 q H 2 O + HSO − 3 + SO 2− 3 ) oxidation by H 2 O 2 in aerosol water accounted for 5-13 % of P het . The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed 17 O(SO 2− 4 ). Heterogeneous sulfate production via S(IV) oxidation by O 3 was estimated to contribute 21-22 % of P het on average. Heterogeneous sulfate production pathways that result in zero-17 O(SO 2− 4 ), such as S(IV) oxidation by NO 2 in aerosol water and/or by O 2 via a radical chain mechanism, contributed the remaining 66-73 % of P het . The assumption about the thermodynamic state of aerosols (stable or metastable) was found to significantly influence the calculated aerosol pH (7.6 ± 0.1 or 4.7 ± 1.1, respectively), and thus influence the relative importance of heterogeneous sulfate production via S(IV) oxidation by NO 2 and by O 2 . Our local atmospheric conditions-based calculations suggest sulfate formation via NO 2 oxidation can be the dominant pathway in aerosols at high-pH conditions calculated assuming stable state while S(IV) oxidation by O 2 can be the dominant pathway providing that highly acidic aerosols (pH ≤ 3) exist. Our local atmospheric-conditions-based calculations illustrate the utility of 17 O(SO 2− 4 ) for quantifying sulfate forPublished by Copernicus Publications on behalf of the European Geosciences Union. 5516 P. He et al.: Isotopic constraints on heterogeneous sulfate production in Beijing haze mation pathways, but this estimate may be further improved with future regional modeling work.

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Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes

Cited by 24 publications

References 64 publications

Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

A review of current knowledge concerning PM<sub>2. 5</sub> chemical composition, aerosol optical properties and their relationships across China

Isotopic constraints on heterogeneous sulfate production in Beijing haze

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Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes

Cited by 24 publications

References 64 publications

Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

Investigating Source Contributions of Size‐Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

A review of current knowledge concerning PM&lt;sub&gt;2. 5&lt;/sub&gt; chemical composition, aerosol optical properties and their relationships across China

Isotopic constraints on heterogeneous sulfate production in Beijing haze

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A review of current knowledge concerning PM<sub>2. 5</sub> chemical composition, aerosol optical properties and their relationships across China