Hattori Shohei, Iizuka Yoshinori, Alexander Becky, Ishino Sakiko, Fujita Koji, Zhai Shuting, Sherwen Tomás, Oshima Naga, Uemura Ryu, Yamada Akinori, Suzuki Nozomi, Matoba Sumito, Tsuruta Asuka, Savarino Joel, Yoshida Naohiro
Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, Yokohama 226-8502, Japan.
Institute of Low Temperature Science, Hokkaido University, Sapporo 060-0819, Japan.
Sci Adv. 2021 May 5;7(19). doi: 10.1126/sciadv.abd4610. Print 2021 May.
After the 1980s, atmospheric sulfate reduction is slower than the dramatic reductions in sulfur dioxide (SO) emissions. However, a lack of observational evidence has hindered the identification of causal feedback mechanisms. Here, we report an increase in the oxygen isotopic composition of sulfate ([Formula: see text]) in a Greenland ice core, implying an enhanced role of acidity-dependent in-cloud oxidation by ozone (up to 17 to 27%) in sulfate production since the 1960s. A global chemical transport model reproduces the magnitude of the increase in observed [Formula: see text] with a 10 to 15% enhancement in the conversion efficiency from SO to sulfate in Eastern North America and Western Europe. With an expected continued decrease in atmospheric acidity, this feedback will continue in the future and partially hinder air quality improvements.
20世纪80年代以后，大气中硫酸盐的减少速度比二氧化硫（SO）排放量的急剧减少速度要慢。然而，缺乏观测证据阻碍了对因果反馈机制的识别。在此，我们报告了格陵兰冰芯中硫酸盐（[公式：见正文]）的氧同位素组成增加，这意味着自20世纪60年代以来，臭氧在酸度依赖的云内氧化过程（高达17%至27%）在硫酸盐生成中发挥了更大作用。一个全球化学传输模型再现了观测到的[公式：见正文]增加幅度，北美东部和西欧从SO转化为硫酸盐的效率提高了10%至15%。随着大气酸度预计将持续下降，这种反馈在未来将继续存在，并部分阻碍空气质量的改善。
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