pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol

Acidity (pH) plays a key role in the physical and chemical behavior of PM_2.5. However, understanding of how specific PM sources impact aerosol pH is rarely considered. Performing source apportionment of PM_2.5 allows a unique link of sources pH of aerosol from the polluted city. Hourly water-soluble (WS) ions of PM_2.5 were measured online from December 25th, 2014 to June 19th, 2015 in a northern city in China. Five sources were resolved including secondary nitrate (41%), secondary sulfate (26%), coal combustion (14%), mineral dust (11%), and vehicle exhaust (9%). The influence of source contributions to pH was estimated by ISORROPIA-II. The lowest aerosol pH levels were found at low WS-ion levels and then increased with increasing total ion levels, until high ion levels occur, at which point the aerosol becomes more acidic as both sulfate and nitrate increase. Ammonium levels increased nearly linearly with sulfate and nitrate until approximately 20 μg m^-3, supporting that the ammonium in the aerosol was more limited by thermodynamics than source limitations, and aerosol pH responded more to the contributions of sources such as dust than levels of sulfate. Commonly used pH indicator ratios were not indicative of the pH estimated using the thermodynamic model.