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Enhanced Sulfate Production by Nitrate Photolysis in the Presence of Halide Ions in Atmospheric Particles.
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-03-03 , DOI: 10.1021/acs.est.9b06445 Ruifeng Zhang 1 , Masao Gen 1, 2 , Dandan Huang 3 , Yongjie Li 4 , Chak K Chan 1
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-03-03 , DOI: 10.1021/acs.est.9b06445 Ruifeng Zhang 1 , Masao Gen 1, 2 , Dandan Huang 3 , Yongjie Li 4 , Chak K Chan 1
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Heterogeneous oxidation of SO2 is an effective production pathway of sulfate in the atmosphere. We recently reported a novel pathway for the heterogeneous oxidation of SO2 by in-particle oxidants (OH, NO2 and NO2-/HNO2) produced from particulate nitrate photolysis (Environ. Sci. Technol. 2019, 53, 8757-8766). Particulate nitrate is often found to coexist with chloride and other halide ions, especially in aged sea-salt aerosols and combustion aerosols. Reactive uptake experiments of SO2 with UV-irradiated nitrate particles showed that sulfate production rates were enhanced by a factor of 1.4, 1.3, and 2.0 in the presence of Cl-, Br-, and I-, respectively, compared to those in the absence of halide ions. The larger sulfate production was attributed to enhanced nitrate photolysis promoted by the increased incomplete solvation of nitrate at the air-particle interface due to the presence of surface-active halide ions. Modeling results based on the experimental data show that the nitrate photolysis rate constants increase by a factor of 2.0, 1.7, and 3.7 in the presence of Cl-, Br-, and I-, respectively. A linear relation was found between the nitrate photolysis rate constant, jNO3-, and the initial molar ratio of Cl- to NO3-, [Cl-]0/[NO3-]0, as jNO3-=9.7×10-5[Cl-]0/[NO3-]0 + 1.9×10-5 at [Cl-]0/[NO3-]0 below 0.2. The present study demonstrates that the presence of halide ions enhances sulfate production produced during particulate nitrate photolysis and provides insights into the enhanced formation of in-particle oxidants that may increase atmospheric oxidative capacity.
中文翻译：
大气颗粒中存在卤化物离子时，硝酸盐光解可提高硫酸盐的生产量。
SO2的异质氧化是大气中硫酸盐的有效生产途径。我们最近报道了一种由微粒硝酸盐光解产生的颗粒内氧化剂（OH，NO2和NO2- / HNO2）进行SO2异质氧化的新途径（Environ.Sci.Technol.2019，53，8757-8766）。经常发现微粒硝酸盐与氯离子和其他卤离子共存，特别是在老化的海盐气溶胶和燃烧气溶胶中。用紫外线照射的硝酸盐颗粒对SO2的反应吸收实验表明，与不存在Cl-，Br-和I-时相比，硫酸盐的生产率分别提高了1.4、1.3和2.0倍。卤离子。由于表面活性卤离子的存在，硝酸盐在空气-颗粒界面处增加的不完全溶解增加，从而促进了硝酸盐的光解，这是硫酸盐产量增加的原因。基于实验数据的建模结果表明，在存在Cl-，Br-和I-的情况下，硝酸盐光解速率常数分别增加了2.0、1.7和3.7倍。发现硝酸盐光解速率常数jNO3-与Cl-与NO3-的初始摩尔比[Cl-] 0 / [NO3-] 0之间存在线性关系，即jNO3- = 9.7×10-5 [Cl -] 0 / [NO3-] 0 + 1.9×10-5在[Cl-] 0 / [NO3-] 0低于0.2的情况下。
更新日期：2020-03-12
中文翻译：
大气颗粒中存在卤化物离子时，硝酸盐光解可提高硫酸盐的生产量。
SO2的异质氧化是大气中硫酸盐的有效生产途径。我们最近报道了一种由微粒硝酸盐光解产生的颗粒内氧化剂（OH，NO2和NO2- / HNO2）进行SO2异质氧化的新途径（Environ.Sci.Technol.2019，53，8757-8766）。经常发现微粒硝酸盐与氯离子和其他卤离子共存，特别是在老化的海盐气溶胶和燃烧气溶胶中。用紫外线照射的硝酸盐颗粒对SO2的反应吸收实验表明，与不存在Cl-，Br-和I-时相比，硫酸盐的生产率分别提高了1.4、1.3和2.0倍。卤离子。由于表面活性卤离子的存在，硝酸盐在空气-颗粒界面处增加的不完全溶解增加，从而促进了硝酸盐的光解，这是硫酸盐产量增加的原因。基于实验数据的建模结果表明，在存在Cl-，Br-和I-的情况下，硝酸盐光解速率常数分别增加了2.0、1.7和3.7倍。发现硝酸盐光解速率常数jNO3-与Cl-与NO3-的初始摩尔比[Cl-] 0 / [NO3-] 0之间存在线性关系，即jNO3- = 9.7×10-5 [Cl -] 0 / [NO3-] 0 + 1.9×10-5在[Cl-] 0 / [NO3-] 0低于0.2的情况下。
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