Extensive field evidence for the release of HONO from the photolysis of nitrate aerosols.

Extensive field evidence for the release of HONO from the photolysis of nitrate aerosols.
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DOI:
10.1126/sciadv.add6266
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发表时间:
2023-01-18
期刊:
影响因子:
13.6
通讯作者:
--
中科院分区:
综合性期刊1区
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--
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长期以来,硝酸盐颗粒()一直被认为是氮氧化物(NO和NO2)的永久汇,可以清除一种对空气质量至关重要并影响大气全球自净能力的气态污染物。越来越多的证据表明,光解可以将HONO和NOx再循环回气相,对对流层臭氧和OH预算具有潜在的重要影响;然而,“再氧化”光解速率常数存在实质性差异。利用飞机和地面在遥远的大西洋对流层的HONO观测,我们展示了在混合海洋气溶胶上发生再氧化作用的证据,其效率随相对湿度的增加而增加,随浓度的降低而降低,从而在很大程度上调和了在多个实验室和实地研究中发现的再氧化光解速率常数的巨大差异。在污染环境和清洁环境中,气溶胶中HONO的主动释放对OH和O3等大气氧化剂具有重要意义。在遥远的大西洋对流层的飞机观测显示了在各种气溶胶类型上产生HONO的证据。
Particulate nitrate () has long been considered a permanent sink for NOx (NO and NO2), removing a gaseous pollutant that is central to air quality and that influences the global self-cleansing capacity of the atmosphere. Evidence is emerging that photolysis of can recycle HONO and NOx back to the gas phase with potentially important implications for tropospheric ozone and OH budgets; however, there are substantial discrepancies in “renoxification” photolysis rate constants. Using aircraft and ground-based HONO observations in the remote Atlantic troposphere, we show evidence for renoxification occurring on mixed marine aerosols with an efficiency that increases with relative humidity and decreases with the concentration of , thus largely reconciling the very large discrepancies in renoxification photolysis rate constants found across multiple laboratory and field studies. Active release of HONO from aerosol has important implications for atmospheric oxidants such as OH and O3 in both polluted and clean environments. Aircraft observations in the remote Atlantic troposphere show evidence for HONO production occurring on various aerosol types.
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