Chemical characteristics of wintertime aerosol and cloud over the Sea of Japan based on aircraft and ground measurements

Chemical characteristics of wintertime aerosol and cloud over the Sea of Japan based on aircraft and ground measurements
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基于飞机和地面测量的日本海冬季气溶胶和云的化学特征

DOI:
10.1016/j.apr.2023.101650
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发表时间:
2023
影响因子:
4.5
通讯作者:
Ishizaka Yutaka
Ishizaka Yutaka
中科院分区:
环境科学与生态学3区
文献类型:
--
作者:
Kagawa Masako;Katsuta Nagayoshi;Nagao Ippei;Aryal Deepak;Ishizaka Yutaka

文献摘要

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在冬季,对日本海上空从边界层到对流层中层(0-5.2 km)的气溶胶和云的化学特征进行了调查,结果表明受到从西伯利亚吹来的亚洲冬季季风的影响。气溶胶和云的 Na+/Cl− 比率表明大多数 Na+ 和 Cl− 来自海盐。研究发现,海浪喷雾气溶胶产生通量与边界层气溶胶(R2=0.53-0.71)或云(R2=0.45-0.69)的(Na++Cl−)浓度呈正相关,这表明强烈的冬季季风加剧了初级海盐和相关云的产生。近地面气溶胶的 Cl 损失程度高于高海拔地区,可能与排放源距离较远有关,而云几乎不伴随 Cl 损失。与自由对流层相比,边界层中气溶胶的 (NO3−+ 非海盐 (nss)-SO42–)/(NH4++ nss-Ca2+) 比率较高,可能归因于相对湿度对气溶胶吸收酸性气体(SO2、H2SO4 和 HNO3)的影响。云的 (NO3−+ nss-SO42–)/(NH4++ nss-Ca2+) 比率(平均 0.67)意味着碱离子数量不足以中和酸离子。边界层气溶胶的Se(VI)/Se(IV)比值大多高于自由对流层,这可能与气溶胶颗粒中硒的氧化剂浓度有关。云中的 Se(IV)/Se(VI) 比率 (1.34 ± 0.62) 与气溶胶的比率 (边界层为 0.50 ± 0.32,自由对流层为 27.92 ± 52.42) 存在显着差异,这强烈表明云中 Se 的氧化态表明氧化还原平衡。
Chemical characteristics of aerosols and clouds from the boundary layer to the middle troposphere (0–5.2 km) were investigated over the Sea of Japan during winter seasons and were shown to be influenced by the Asian winter monsoon blowing from Siberia. The Na+/Cl−ratio of aerosols and clouds indicates that most Na+and Cl−originated from sea salts. Positive correlations were found between sea spray aerosol production flux and (Na++ Cl−) concentrations of boundary layer aerosols (R2= 0.53–0.71) or clouds (R2= 0.45–0.69), suggesting that strong winter monsoon winds intensified the production of primary sea salts and the associated clouds. The degree of Cl loss for aerosols near ground level was higher than that at high altitudes, which may be attributed to the distance from emission sources, whereas clouds were scarcely accompanied by Cl loss. The higher (NO3−+ non-sea salt (nss)-SO42–)/(NH4++ nss-Ca2+) ratio of aerosols in the boundary layer compared with the free troposphere may be attributed to the effect of relative humidity on acid gases (SO2, H2SO4, and HNO3) uptake to aerosols. The (NO3−+ nss-SO42–)/(NH4++ nss-Ca2+) ratio of clouds (0.67 on average) implies insufficient amounts of base ions to neutralize acid ions. The Se(VI)/Se(IV) ratios of aerosols in the boundary layer were mostly higher than those of the free troposphere, which may be attributed to the concentrations of oxidants for selenium in aerosol particles. The Se(IV)/Se(VI) ratios of clouds (1.34 ± 0.62) were found to differ significantly from those of aerosols (0.50 ± 0.32 for the boundary layer, 27.92 ± 52.42 for the free troposphere), which strongly suggests that the oxidation state of Se in cloud indicates redox equilibrium.