Isotopic evidence for acidity-driven enhancement of sulfate formation after SO<sub>2</sub> emission control.

Hattori, Shohei; Iizuka, Yoshinori; Alexander, Becky; Ishino, Sakiko; Fujita, Koji; Zhai, Shuting; Sherwen, Tomás; Oshima, Naga et al. · Sci Adv · 2021

basic_science · Level V

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Abstract

After the 1980s, atmospheric sulfate reduction is slower than the dramatic reductions in sulfur dioxide (SO<sub>2</sub>) 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<sub>2</sub> 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.