Multiple oxygen and sulfur isotope compositions of secondary atmospheric sulfate in a mega-city in central China

Li, Xiaoqian; Bao, Huiming; Gan, Yiqun; Zhou, Aiguo; Liu, Yunde

doi:10.1016/j.atmosenv.2013.09.051

Cited by 45 publications

(38 citation statements)

References 59 publications

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“…Atmospheric H 2 SO 4 and HNO 3 could have been formed, resulting in the Cl À deficit in sea-salt aerosols and the increase of atmospheric HCl (Koehler and Wassenaar, 2010;Volpe et al, 1998). Several studies using d 34 S and d 18 O evidences also proved the significant input of atmospheric SO 2À 4 due to pollution in China (Bai and Wang, 2014;Li et al, 2013a;Xiao et al, 2009). Accordingly, the contribution of tropospheric HCl derived from acidification of sea-salt aerosol was proposed to be the most likely reason for the negative d 37 Cl values of these samples.…”

Section: Sources Of Chloride In the Surface Water And Groundwatermentioning

confidence: 95%

Application of hydrochemistry and stable isotopes (δ34S, δ18O and δ37Cl) to trace natural and anthropogenic influences on the quality of groundwater in the piedmont region, Shijiazhuang, China

Zhou

Zhang

Zhou

et al. 2016

Applied Geochemistry

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Section: Sources Of Chloride In the Surface Water And Groundwatermentioning

confidence: 95%

Application of hydrochemistry and stable isotopes (δ34S, δ18O and δ37Cl) to trace natural and anthropogenic influences on the quality of groundwater in the piedmont region, Shijiazhuang, China

Zhou

Zhang

Zhou

et al. 2016

Applied Geochemistry

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“…5c). The mean value of 17 O cloud calculated here is close to 17 O(SO 2− 4 ) in rainwater observed in central China (0.53 ± 0.19 ‰) (Li et al, 2013) and at Baton Rouge, USA (0.62 ± 0.32 ‰) (Jenkins and Bao, 2006). In addition, by using Eq.…”

Section: Chemical Kinetic Calculations With the Constraint Of 17 O Obsmentioning

confidence: 99%

“…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%

“…The primary sulfate, which is directly emitted into air, includes the sea salt source, terrigenous source, and anthropogenic source (Li et al, 2013;Faloona, 2009). The concentration of sea salt sulfate was calculated by using the observed concentrations of Na + and the mass ratio of c(SO 2− 4 ) / c(Na + ) = 0.252 in seawater (Calhoun et al, 1991).…”

Section: Estimate Of Primary Sulfatementioning

confidence: 99%

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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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“…The primary sulfate, which is directly emitted into air, includes the sea salt source, terrigenous source and 132 anthropogenic source (Li et al, 2013;Faloona, 2009). The concentration of sea salt sulfate was calculated by using the 133 observed concentrations of SO 4 2-and Na + and the mass ratio of (SO 4 2-/Na + ) = 0.252 in seawater (Calhoun et al, 1991).…”

Section: Estimate Of Primary Sulfate 131mentioning

confidence: 99%

Isotopic constraints on heterogeneous sulphate production in Beijing haze

He¹,

Alexander²,

Geng³

et al. 2017

Preprint

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Abstract. Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter)in Beijing 16 is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. 17Here we present the first observations of the oxygen-17 excess of PM 2.5 sulfate (Δ 17 O(SO 4 2-)) collected in Beijing haze from 18October 2014 to January 2015, to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 19 12h-averaged PM 2.5 concentrations ranged from 16 to 323 μg m -3 with a mean of (141±88 (1σ)

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Multiple oxygen and sulfur isotope compositions of secondary atmospheric sulfate in a mega-city in central China

Cited by 45 publications

References 59 publications

Application of hydrochemistry and stable isotopes (δ34S, δ18O and δ37Cl) to trace natural and anthropogenic influences on the quality of groundwater in the piedmont region, Shijiazhuang, China

Application of hydrochemistry and stable isotopes (δ34S, δ18O and δ37Cl) to trace natural and anthropogenic influences on the quality of groundwater in the piedmont region, Shijiazhuang, China

Isotopic constraints on heterogeneous sulfate production in Beijing haze

Isotopic constraints on heterogeneous sulphate production in Beijing haze

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