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Quantifying SO.sub.2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation

Atmospheric chemistry and physics, 2024-02, Vol.24 (4), p.2195 [Peer Reviewed Journal]

COPYRIGHT 2024 Copernicus GmbH ;ISSN: 1680-7316 ;EISSN: 1680-7324

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  • Title:
    Quantifying SO.sub.2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation
  • Author: Guo, Ziyan ; Lu, Keding ; Qiu, Pengxiang ; Xu, Mingyi ; Guo, Zhaobing
  • Subjects: Oxidation-reduction reaction ; Sulfates
  • Is Part Of: Atmospheric chemistry and physics, 2024-02, Vol.24 (4), p.2195
  • Description: The formation of secondary sulfate in the atmosphere remains controversial, and it is an urgent need to seek a new method to quantify different sulfate formation pathways. Thus, SO.sub.2 and PM.sub.2.5 samples were collected from 4 to 22 December 2019 in the Nanjing region. Sulfur and oxygen isotopic compositions were synchronously measured to study the contribution of SO.sub.2 homogeneous and heterogeneous oxidation to sulfate. Meanwhile, the correlation of [delta].sup.18 O values between H.sub.2 O and sulfate from SO.sub.2 oxidation by H.sub.2 O.sub.2 and Fe.sup.3+ / O.sub.2 was simulatively investigated in the laboratory. Based on isotope mass equilibrium equations, the ratios of different SO.sub.2 oxidation pathways were quantified. The results showed that secondary sulfate constituted higher than 80 % of total sulfate in PM.sub.2.5 during the sampling period. Laboratory simulation experiments indicated that the [delta].sup.18 O value of sulfate was linearly dependent on the [delta].sup.18 O value of water, and the slopes of linear curves for SO.sub.2 oxidation by H.sub.2 O.sub.2 and Fe.sup.3+ / O.sub.2 were 0.43 and 0.65, respectively. The secondary sulfate in PM.sub.2.5 was mainly ascribed to SO.sub.2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H.sub.2 O.sub.2 and Fe.sup.3+ / O.sub.2 . SO.sub.2 heterogeneous oxidation was generally dominant during sulfate formation, and SO.sub.2 oxidation by H.sub.2 O.sub.2 predominated in SO.sub.2 heterogeneous oxidation reactions, with an average ratio around 54.6 %. This study provided an insight into precisely evaluating sulfate formation by combining stable sulfur and oxygen isotopes.
  • Publisher: Copernicus GmbH
  • Language: English
  • Identifier: ISSN: 1680-7316
    EISSN: 1680-7324
  • Source: GFMER Free Medical Journals
    Alma/SFX Local Collection
    ProQuest Central
    DOAJ Directory of Open Access Journals
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