沿海城市地区尺寸分辨海盐气溶胶的酸度：现有方法和新方法的比较,ACS Earth and Space Chemistry

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沿海城市地区尺寸分辨海盐气溶胶的酸度：现有方法和新方法的比较
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2022-04-25 , DOI: 10.1021/acsearthspacechem.1c00367
Ye Tao ₁ , Alexander Moravek ₁ , Teles C. Furlani ₁ , Cameron E. Power ₂ , Trevor C. VandenBoer ₁ , Rachel Y.-W. Chang ₃ , Aldona Wiacek ₂ , Cora J. Young _{1,

4}

Affiliation

2019 年初夏，在加拿大哈利法克斯雾和空气质量研究 (HaliFAQS) 实地活动中监测和研究了海盐气溶胶的老化和 HCl/Cl 的相应相分配行为。^来自环境气溶胶的离子化学成分对10 nm的总悬浮颗粒（TSPs）进行采样并测量14个尺寸范围，表明采样位置的气溶胶主要由海盐成分组成，受次生无机前体人为排放的影响较小。_{通过扩展气溶胶无机模型 (E-AIM) IV 和基于 NH 3} /NH ₄⁺和 HNO ₃ /NO测量的新衍生方法计算老化海盐气溶胶的尺寸分辨 pH₃^–或 HCl/Cl ^–耦合相分配行为。后一种 pH 计算方法不需要有关气溶胶液体水含量的信息或完整的水溶性离子测量，从而补偿了氧化有机物对质子活性的影响。相比之下，E-AIM 计算需要输入所有主要吸湿性物质。_{通过 E-AIM IV 计算的尺寸分辨 pH 通常与通过 NH 3} -HCl 耦合相分配计算的 pH 值一致。_{HCl和HNO 3}的敏感性用观测数据和概念模型研究了气溶胶 pH 的相分配，这提供了证据表明，_在颗粒通常具有 pH > 3. 更高的浓度和更可靠的测量也使 HCl 成为本研究中跟踪 pH 变化的更合适的选择。

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Acidity of Size-Resolved Sea-Salt Aerosol in a Coastal Urban Area: Comparison of Existing and New Approaches

Aging of sea-salt aerosol and the corresponding phase partitioning behavior of HCl/Cl^– were monitored and studied in the Halifax Fog and Air Quality Study (HaliFAQS) field campaign in Canada in the early summer of 2019. Ionic chemical composition of ambient aerosol from total suspended particles (TSPs) to 10 nm was sampled and measured into 14 size ranges, which showed that aerosol at the sampling location was mainly composed of sea-salt constituents with little influence from anthropogenic emissions of secondary inorganic precursors. The size-resolved pH of aged sea-salt aerosol was calculated by Extended Aerosol Inorganic Model (E-AIM) IV and a newly derived method based on the measurement of NH₃/NH₄⁺ and HNO₃/NO₃^– or HCl/Cl^– coupled phase partitioning behavior. The latter pH calculation method does not require information about the aerosol liquid water content or complete water-soluble ion measurement, compensating for the role of oxidized organics to influence the proton activity. In comparison, E-AIM calculation requires the input of all major hygroscopic species. The size-resolved pH calculated by E-AIM IV generally agrees with the one calculated by NH₃–HCl coupled phase partitioning. The sensitivities of HCl and HNO₃ phase partitioning to aerosol pH are studied with both observational data and conceptual modeling, which gives evidence that the phase partitioning of HCl is more sensitive and therefore more reflective of aerosol pH changes than HNO₃ in sea-salt dominated atmospheres where particles typically have pH > 3. The higher concentration and more reliable measurement also make HCl a more suitable choice to track pH changes in this study.

更新日期：2022-04-25

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