Millet Dylan B, Baasandorj Munkhbayar, Hu Lu, Mitroo Dhruv, Turner Jay, Williams Brent J
University of Minnesota , St. Paul, Minnesota 55108, United States.
Washington University in St. Louis , St. Louis, Missouri 63130, United States.
Environ Sci Technol. 2016 Apr 19;50(8):4335-42. doi: 10.1021/acs.est.5b06367. Epub 2016 Apr 7.
Isoprene is the predominant non-methane volatile organic compound emitted to the atmosphere and shapes tropospheric composition and biogeochemistry through its effects on ozone, other oxidants, aerosols, and the nitrogen cycle. Isoprene is emitted naturally by vegetation during daytime, when its photo-oxidation is rapid, and in the presence of nitrogen oxides (NOx) produces ozone and degrades air quality in polluted regions. Here, we show for a city downwind of an isoprene-emitting forest (St. Louis, MO) that isoprene actually peaks at night; ambient levels then endure, owing to low nighttime OH radical concentrations. Nocturnal chemistry controls the fate of that isoprene and the likelihood of a high-ozone episode the following day. When nitrate (NO3) radicals are suppressed, high isoprene persists through the night, providing photochemical fuel upon daybreak and leading to a dramatic late-morning ozone peak. On nights with significant NO3, isoprene is removed before dawn; days with low morning isoprene then have lower ozone with a more typical afternoon peak. This biogenic-anthropogenic coupling expands the daily high-ozone window and likely has an opposite O3-NOx response to what would otherwise be expected, with implications for exposure and air-quality management in cities that, like St. Louis, are downwind of major isoprene-emitting forests.
异戊二烯是排放到大气中的主要非甲烷挥发性有机化合物,它通过对臭氧、其他氧化剂、气溶胶和氮循环的影响塑造对流层的组成和生物地球化学。异戊二烯在白天由植被自然排放,此时其光氧化作用迅速,并且在氮氧化物(NOx)存在的情况下会产生臭氧并降低污染地区的空气质量。在此,我们针对一个位于异戊二烯排放森林下风处的城市(密苏里州圣路易斯)表明,异戊二烯实际上在夜间达到峰值;由于夜间OH自由基浓度较低,其环境水平随后持续存在。夜间化学过程控制着该异戊二烯的归宿以及次日出现高臭氧事件的可能性。当硝酸根(NO3)自由基受到抑制时,高浓度的异戊二烯会整夜持续存在,在黎明时分提供光化学燃料并导致上午晚些时候出现显著的臭氧峰值。在有大量NO3的夜晚,异戊二烯在黎明前被清除;次日上午异戊二烯含量低时,臭氧含量也较低,且下午峰值更为典型。这种生物源 - 人为源的耦合拓宽了每日高臭氧时段,并且可能对O3 - NOx的响应与预期情况相反,这对像圣路易斯这样位于主要异戊二烯排放森林下风处的城市的暴露情况和空气质量管理具有影响。