Isotopic comparison of ammonium between two summertime field campaigns in 2013 and 2021 at a background site of North China

Abstract

Ammonia (NH3) is the primary atmospheric alkaline gas, playing a crucial role in the atmospheric chemistry. Recently, non-agricultural emissions have been identified as the dominant sources of NH3 in urban areas. However, few studies have quantified the contributions of different sources to regional NH3. This study conducted two summertime field observations in 2013 and 2021 at a background site of North China to comprehensively explore the regional variations in concentration, nitrogen isotope composition (δ15N), and sources of ammonium (NH4+). The results indicate that NHx (NHx = NH3 + NH4+) concentration has increased in 2021, but the fNH4+ (NH4+/ NHx) has decreased significantly. The δ15N-NH4+ values show a significant increase, ranging from −4.7 ± 8.1 ‰ to +12.0 ± 2.4 ‰. The increase can be attributed to two primary factors: changes in fNH4+ resulting from the reduction of atmospheric acid gases and alterations in the sources of NH3. Bayesian simulation analysis reveals substantial variations in NH3 sources between 2013 and 2021 observations. Non-agricultural sources have significantly increased their contribution to NHx concentration, with vehicle exhaust and NH3 slip experiencing growth rates of 187 % and 104 %, respectively. Our results confirm the dominate contribution of non-agricultural sources to regional NH3 at the present stage and propose relevant mitigation strategies, which would provide essential insights for reducing NH3 emissions in North China.