Source apportionment and evolution of N-containing aerosols at a rural cloud forest in Taiwan by isotope analysis

Ammonium and nitrate are major N-containing aerosol components. The deposition of N-containing aerosols has impacts on regional ecology and the biogeochemical cycle. In this study, aerosols in a rural cloud forest (Xitou in Taiwan) were studied using 15N and 18O isotope analysis to assess the sources and formation pathways of the local N-containing aerosols linking to a metropolitan. Aerosol samples of different size ranges were collected using a micro-orifice uniform deposit impactor (MOUDI) on a half-day basis in December 2018. The chemical functional groups were analyzed using a Fourier-transform infrared spectroscopy with attenuated total reflection (FTIR-ATR) technique, while the isotope analysis was performed using a gas chromatography–isotope ratio mass spectrometer (GC–IRMS). The average measured aerosol concentration (PM10) was 0.98 (ranging from 0.15 to 3.31) and 0.25 (ranging from 0.00 to 1.51) µg m−3 for NH4+ and NO3-, respectively. In general, a higher concentration than nighttime was observed during the daytime by a factor of 1.5–6, likely due to the transportation of pollutants from upper-stream urban and industrial regions through the local sea breeze combined with valley wind. The presence of fog can further elevate the concentration by a factor of 2–3, resulting from the stronger inversion and lower boundary layer height. The higher NH4+ concentration in fine particles under foggy conditions corresponds to submicron-sized NO3- formation via aqueous-phase dissolution with NH4+ neutralization. Furthermore, the higher RH during fog events shifted the mass distribution of aerosol functional groups to a larger mode size. By comparing the δ15N value directly or through the analysis using a statistical isotope mixing model, MixSIAR, NH4+ probably originated from the industries, coal-fired power plants (CFPPs), or fertilizer plants, while NO3- might be contributed from the CFPP, industrial or urban sources. The overall δ18O of NO3- is +72.66 ‰ ± 3.42 ‰, similar to that in other winter Asian studies, suggesting the major formation pathway via O3 oxidation (δ18O=+72.5 ‰ to 101.67 ‰). However, a lower δ18O (