Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts
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Abstract. Atmospheric measurements showed rapid sulfate formation during severe haze episodes in China, with fine particulate matter (PM) consisting of a multi-component mixture that is dominated by organic species. Several recent studies using the thermodynamic model estimated the particle acidity and sulfate production rate, by treating the PM exclusively as a mixture of inorganic salts dominated by ammonium sulfate and neglecting the effects of organic compounds. Noticeably, the estimated pH and sulfate formation rate during pollution periods in China were highly conflicting among the previous studies. Here we show that a particle mixture of inorganic salts adopted by the previous studies does not represent a suitable model system and that the acidity and sulfate formation cannot be reliably inferred without accounting for the effects of multi-aerosol compositions during severe haze events in China. Our laboratory experiments show that SO2 oxidation by NO2 with NH3 neutralization on fine aerosols is dependent on the particle hygroscopicity, phase-state, and acidity. Ammonium sulfate and oxalic acid seed particles exposed to vapors of SO2, NO2, and NH3 at high relative humidity (RH) exhibit distinct size growth and sulfate formation. Aqueous ammonium sulfate particles exhibit little sulfate production because of high acidity, in contrast to aqueous oxalic acid particles with significant sulfate production because of low acidity. Our field measurements demonstrate significant contribution of water-soluble organic matter to fine PM in China and indicate that the use of oxalic acid in laboratory experiments is representative of ambient organic dominant aerosols. While the particle acidity cannot be accurately determined from field measurements or calculated using the thermodynamic model, our results reveal that the pH value of ambient organics-dominated aerosols is sufficiently high to promote efficient SO2 oxidation by NO2 with NH3 neutralization under polluted conditions in China.
