Institute of Surface-Earth System Science, Tianjin University, Tianjin, 300072, China.
Institute of Surface-Earth System Science, Tianjin University, Tianjin, 300072, China; State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, 550002, China.
Environ Pollut. 2018 Aug;239:392-398. doi: 10.1016/j.envpol.2018.04.015. Epub 2018 Apr 17.
Enhanced ammonia (NH) emissions and deposition caused negative effects on air quality and ecosystems. Precipitation is an efficient pathway to remove NH and particulate ammonium (p-NH) from the atmosphere into ecosystems. However, precipitation scavenging of p-NH in chemical transport models has often considered fine p-NH, with inadequate constraints on NH and coarse p-NH. Based on distinct δN values between NH and NH in PM (particulate matters with aerodynamic diameters ≤ 2.5 μm) or TSP (total suspended particulates), this paper interpreted intra-event variations of precipitation NH concentrations and δN values (δN-NH values) at Guiyang (Xiao et al., 2015). Generally decreased NH concentrations across rain events reflected decreasing scavenging of NH and p-NH. Using a Bayesian isotope mixing model, we found that differing contributions between N-depleted NH and N-enriched p-NH were responsible for the three-stage variations of intra-event δN-NH values. The decreases of δN-NH values across the first and third stages indicated more decreases in scavenging p-NH than NH, while the increases of δN-NH values across the second stage were resulted primarily from more increases in scavenging p-NH (particularly fine p-NH) than NH. These results stressed influences of differing scavenging between NH and p-NH on precipitation δN-NH values, which should be considered in modeling precipitation scavenging of atmospheric p-NH.
增强的氨(NH)排放和沉积对空气质量和生态系统产生了负面影响。降水是将大气中的 NH 和颗粒态铵(p-NH)有效去除并输入到生态系统中的途径之一。然而,在化学输送模型中,降水对 p-NH 的去除往往仅考虑了细颗粒态 p-NH,而对 NH 和粗颗粒态 p-NH 的约束不足。本研究基于 PM(空气动力学直径≤2.5μm 的颗粒物)或 TSP(总悬浮颗粒物)中 NH 和 NH 的独特 δN 值,解释了贵阳降水 NH 浓度和 δN 值(δN-NH 值)的事件内变化(Xiao 等人,2015 年)。整个降水事件中 NH 浓度的普遍降低反映了 NH 和 p-NH 去除效率的降低。利用贝叶斯同位素混合模型,我们发现 N 贫化的 NH 和 N 富化的 p-NH 之间的不同贡献是导致事件内 δN-NH 值三阶段变化的原因。第一和第三阶段 δN-NH 值的降低表明 p-NH 的去除效率比 NH 降低得更快,而第二阶段 δN-NH 值的增加主要是由于 p-NH(尤其是细颗粒态 p-NH)的去除效率比 NH 增加得更快。这些结果强调了 NH 和 p-NH 之间不同去除效率对降水 δN-NH 值的影响,在大气 p-NH 的降水去除模拟中应予以考虑。