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High levels of ammonia do not raise fine particle pH sufficiently to yield nitrogen oxide-dominated sulfate production

2017; Nature Portfolio; Volume: 7; Issue: 1 Linguagem: Inglês

10.1038/s41598-017-11704-0

2045-2322

Hongyu Guo, Rodney J. Weber, Athanasios Nenes,

Air Quality and Health Impacts

Abstract High levels of ammonia (NH 3 ) have been suggested to elevate ambient particle pH levels to near neutral acidity (pH = 7), a condition that promotes rapid SO 2 oxidation by NO 2 to form aerosol sulfate concentration consistent with “London fog” levels. This postulation is tested using aerosol data from representative sites around the world to conduct a thorough thermodynamic analysis of aerosol pH and its sensitivity to NH 3 levels. We find that particle pH, regardless of ammonia levels, is always acidic even for the unusually high NH 3 levels found in Beijing (pH = 4.5) and Xi’an (pH = 5), locations where sulfate production from NO x is proposed. Therefore, major sulfate oxidation through a NO 2 -mediated pathway is not likely in China, or any other region of the world (e.g., US, Mediterranean) where the aerosol is consistently more acidic. The limited alkalinity from the carbonate buffer in dust and seasalt can provide the only likely set of conditions where NO 2 -mediated oxidation of SO 2 outcompetes with other well-established pathways. The mildly acidic levels associated with excessive amounts of ammonia can promote high rates of SO 2 oxidation through transition metal chemistry, this may be an alternative important aerosol chemical contributor to the extreme pollution events.