Impacts of missing OH reactivity and aerosol uptake of HO2 radicals on tropospheric O3 production during the AQUAS-Kyoto summer campaign in 2018
Impacts of missing OH reactivity and aerosol uptake of HO2 radicals on tropospheric O3 production during the AQUAS-Kyoto summer campaign in 2018
复制标题
2018 年 AQUAS-Kyoto 夏季活动期间，OH 反应性缺失和 HO2 自由基气溶胶吸收对对流层 O3 产生的影响
DOI：
10.1016/j.atmosenv.2022.119130
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发表时间：
2022
影响因子：
5
通讯作者：
Y. Kajii
中科院分区：
文献类型：
--
作者：
N. Kohno;J. Zhou;J. Li;M. Takemura;N. Ono;Y. Sadanaga;Y. Nakashima;K. Sato;S. Kato;Y. Sakamoto;Y. Kajii
获得有关HOxcycle参与臭氧（O3）产生的定量信息对于减少对流层臭氧是重要的。在这项研究中，我们评估了在2018年空气质量研究(AQUAS)-京都夏季运动期间，由于环境气溶胶吸收而导致的OH反应性缺失和ho2的异质性损失对光化学臭氧生产潜力和制度分析的影响。我们检测了缺失的OH反应活性，占平均总OH反应活性的50%(9.8 ± 3.8 (1σ) s−1)，以及环境气溶胶对ho2o的吸收损失率为0.0017 ± 0.0015 s−1。采用多用途气溶胶浓度富集系统（VACES）测量了ho2的实时吸收损失率。当考虑到缺乏OH反应性时，臭氧生产潜力增加了2倍，而当考虑到气溶胶吸收造成的ho2损失时，臭氧生产潜力下降了约20%。此外，由于气溶胶吸收导致的OH反应性缺失和ho2损失降低了o3生成速率对挥发性有机化合物（VOCs）的相对敏感性，增加了对NOx（= NO + NO2）的相对敏感性。因此，nox限制期（即臭氧生成速率对nox的相对敏感性高于对VOCs的相对敏感性）延长了几个小时。最后，气溶胶吸收对臭氧生成的影响与NO浓度呈反相关关系，在NO浓度最低的正午前后达到峰值。结论是，气溶胶可能影响郊区和农村地区的对流层臭氧产生，因为这些地区的NOx浓度，特别是NO浓度非常低（[NO] < 0.3 ppb）。
Gaining quantitative information about the HOxcycle involved in ozone (O3) production is important for reduction of tropospheric O3. In this study, we evaluated the impacts of both the missing OH reactivity and the heterogeneous loss of HO2due to ambient aerosol uptake on the photochemical O3production potential and regime analysis during the Air QUAlity Study (AQUAS)-Kyoto summer campaign in 2018. We examined the missing OH reactivity, which was 50% of the averaged total OH reactivity (9.8 ± 3.8 (1σ) s−1), and the uptake loss rate of HO2on ambient aerosols of 0.0017 ± 0.0015 s−1. The real-time uptake loss rate of HO2was measured by employing a versatile aerosol concentration enrichment system (VACES). The O3production potential increased by a factor of two when the missing OH reactivity was considered and decreased by ∼20% when the HO2loss due to aerosol uptake was considered. In addition, the missing OH reactivity and the HO2loss due to aerosol uptake decreased the relative sensitivity of the O3production rate to volatile organic compounds (VOCs) and increased that to NOx(= NO + NO2). Consequently, the NOxlimited regime period, the period in which the relative sensitivity of the O3production rate to NOxwas higher than that to VOCs, was expanded by a few hours. Finally, the effect of aerosol uptake on O3production was anti-correlated with the NO concentration and peaked around noon when the NO concentration was the minimum. It is concluded that aerosols likely affect tropospheric O3production in suburban and rural areas, where the concentrations of NOx, particularly NO, are very low ([NO] < 0.3 ppb).