Importance of gas-particle partitioning of ammonia in haze formation in the rural agricultural environment

Abstract

Ammonia in the atmosphere is essential for the formation of fine particles that impact air quality and climate. Despite extensive prior research to disentangle the relationship between ammonia and haze pollution, the role of ammonia in haze formation in high ammonia-emitting regions is still not well understood. Aiming to better understand secondary inorganic aerosol (sulfate, nitrate, ammonium – SNA) formation mechanisms under high-ammonia conditions, 1-year hourly measurement of water-soluble inorganic species (gas and particle) was conducted at a rural supersite in Shanghai. Exceedingly high levels of agricultural ammonia, constantly around 30 µg m−3, were observed. We find that gas-particle partitioning of ammonia (ε(NH4+)), as opposed to ammonia concentrations, plays a critical role in SNA formation during the haze period. From an assessment of the effects of various parameters, including temperature (T), aerosol water content (AWC), aerosol pH, and activity coefficient, it seems that AWC plays predominant regulating roles for ε(NH4+). We propose a self-amplifying feedback mechanism associated with ε(NH4+) for the formation of SNA, which is consistent with diurnal variations in ε(NH4+), AWC, and SNA. Our results imply that a reduction in ammonia emissions alone may not reduce SNA effectively, at least at rural agricultural sites in China.