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碘辅助气溶胶粒子形成在南极洲的作用。

Role of Iodine-Assisted Aerosol Particle Formation in Antarctica.

机构信息

Department of Physics, Lund University, Professorsgatan 1, Lund SE-22363, Sweden.

Swedish Meteorological and Hydrological Institute (SMHI), Norrköping SE-60176, Sweden.

出版信息

Environ Sci Technol. 2024 Apr 30;58(17):7314-7324. doi: 10.1021/acs.est.3c09103. Epub 2024 Apr 16.

DOI:10.1021/acs.est.3c09103
PMID:38626432
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11064213/
Abstract

New particle formation via the ion-mediated sulfuric acid and ammonia molecular clustering mechanism remains the most widely observed and experimentally verified pathway. Recent laboratory and molecular level observations indicate iodine-driven nucleation as a potentially important source of new particles, especially in coastal areas. In this study, we assess the role of iodine species in particle formation using the best available molecular thermochemistry data and coupled to a detailed 1-d column model which is run along air mass trajectories over the Southern Ocean and the coast of Antarctica. In the air masses traversing the open ocean, ion-mediated SA-NH clustering appears insufficient to explain the observed particle size distribution, wherein the simulated Aitken mode is lacking. Including the iodine-assisted particle formation improves the modeled Aitken mode representation with an increase in the number of freshly formed particles. This implies that more particles survive and grow to Aitken mode sizes via condensation of gaseous precursors and heterogeneous reactions. Under certain meteorological conditions, iodine-assisted particle formation can increase cloud condensation nuclei concentrations by 20%-100%.

摘要

通过离子介导的硫酸和氨分子簇机制形成新粒子仍然是最广泛观察到和经过实验验证的途径。最近的实验室和分子水平的观测表明,碘驱动成核是新粒子形成的一个潜在重要来源,特别是在沿海地区。在这项研究中,我们使用最好的可用分子热化学数据来评估碘物种在颗粒形成中的作用,并将其与详细的 1 维柱模型耦合,该模型沿着大气质量轨迹在南大洋和南极洲海岸上空运行。在穿越开阔海洋的气团中,离子介导的 SA-NH 聚类似乎不足以解释观测到的颗粒尺寸分布,其中模拟的艾肯模式缺失。通过包括碘辅助的颗粒形成,可以通过气态前体的冷凝和多相反应增加新形成的颗粒数量,从而改善模拟的艾肯模式表示。这意味着更多的颗粒通过气态前体的冷凝和多相反应幸存并生长到艾肯模式尺寸。在某些气象条件下,碘辅助的颗粒形成可以使云凝结核浓度增加 20%到 100%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/072f3decdcaf/es3c09103_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/f60e2aed5730/es3c09103_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/e1e0e933c295/es3c09103_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/a1c310c5f5eb/es3c09103_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/b229e19bff3d/es3c09103_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/072f3decdcaf/es3c09103_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/f60e2aed5730/es3c09103_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/e1e0e933c295/es3c09103_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/a1c310c5f5eb/es3c09103_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/b229e19bff3d/es3c09103_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90f9/11064213/072f3decdcaf/es3c09103_0005.jpg

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本文引用的文献

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Science. 2023 Dec 15;382(6676):1308-1314. doi: 10.1126/science.adh2526. Epub 2023 Dec 14.
2
The gas-phase formation mechanism of iodic acid as an atmospheric aerosol source.碘酸作为大气气溶胶源的气相形成机制。
Nat Chem. 2023 Jan;15(1):129-135. doi: 10.1038/s41557-022-01067-z. Epub 2022 Nov 14.
3
Critical Role of Iodous Acid in Neutral Iodine Oxoacid Nucleation.碘酸在中性碘含氧酸成核中的关键作用。
Environ Sci Technol. 2022 Oct 4;56(19):14166-14177. doi: 10.1021/acs.est.2c04328. Epub 2022 Sep 20.
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Role of gas-molecular cluster-aerosol dynamics in atmospheric new-particle formation.气体分子团簇气溶胶动力学在大气新粒子形成中的作用。
Sci Rep. 2022 Jun 16;12(1):10135. doi: 10.1038/s41598-022-14525-y.
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Role of iodine oxoacids in atmospheric aerosol nucleation.碘氧酸在大气气溶胶成核中的作用。
Science. 2021 Feb 5;371(6529):589-595. doi: 10.1126/science.abe0298. Epub 2021 Feb 4.
6
Frequent new particle formation over the high Arctic pack ice by enhanced iodine emissions.高北极海冰上方频繁的新粒子形成归因于碘排放增强。
Nat Commun. 2020 Oct 1;11(1):4924. doi: 10.1038/s41467-020-18551-0.
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Impact of Quantum Chemistry Parameter Choices and Cluster Distribution Model Settings on Modeled Atmospheric Particle Formation Rates.量子化学参数选择和团簇分布模型设置对模拟大气颗粒物形成速率的影响
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Aerosols in the Pre-industrial Atmosphere.工业化前大气中的气溶胶
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Sci Adv. 2018 Nov 28;4(11):eaat9744. doi: 10.1126/sciadv.aat9744. eCollection 2018 Nov.