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Nitric acid dry deposition associated with equilibrium shift of ammonium nitrate above a forest by long-term measurement using relaxed eddy accumulation
Atmospheric Environment ( IF 4.2 ) Pub Date : 2021-05-02 , DOI: 10.1016/j.atmosenv.2021.118454
Mao Xu , Kenta Kasahara , Atsuyuki Sorimachi , Kazuhide Matsuda

The dry deposition process of nitrogen compounds still has considerable uncertainty due to the complex compound behavior in the atmosphere. To enhance understanding of the nitric acid (HNO3) dry deposition process that largely contributes to the total nitrogen deposition, we associate this process with the equilibrium shift of ammonium nitrate (NH4NO3) to HNO3 and ammonia (NH3) near the surface. We obtained the flux of HNO3 and PM2.5 components above a forest in suburban Tokyo using a relaxed eddy accumulation (REA) system incorporating the denuder/filter-pack sampling technique. We conducted continuous samplings on a weekly basis over a long-term period, from October 14, 2016 to October 3, 2018, including leafy and leafless conditions. The measured deposition velocities of fine NO3 particles were significantly (p < 0.05) larger than those of fine SO42− particles and similar to those of HNO3, regardless of the leafy and leafless periods. The larger deposition velocities of fine NO3 particles caused by the equilibrium shift of NH4NO3 were found to be similar to previous measurements at the same site. The measured deposition velocities of HNO3 were low and included many emission cases compared to those of fine NO3 particles. The lower HNO3 deposition velocities were associated with the equilibrium shift of NH4NO3 to the gas phase, causing the suppressed deposition and apparent emission of HNO3, particularly during the leafless period. The emission of HNO3 is possibly due to high HNO3 concentration near the surface, which is attributed to a small removal of the leafless canopy. The turbulence enhanced both the upward and downward fluxes of HNO3. These results will contribute to the better understanding for the dynamics of the nitrogen compounds in the atmosphere and the accurate assessment for the nitrogen deposition.



中文翻译:

长期测量利用松弛涡流积累,硝酸干沉降与森林上方硝酸铵的平衡迁移有关

由于大气中复杂的化合物行为,氮化合物的干法沉积工艺仍具有相当大的不确定性。为了增强对硝酸盐(HNO 3)干式沉积过程的理解,该过程对总氮沉积有很大贡献,我们将此过程与硝酸铵(NH 4 NO 3)到HNO 3和氨(NH 3)附近的平衡位移联系起来。表面。我们获得了HNO 3和PM 2.5的通量使用放松的涡流累积(REA)系统并结合了剥蚀器/滤嘴组采样技术,在东京郊区的一片森林上方收集了一些组件。从2016年10月14日到2018年10月3日,我们在长期内每周进行连续采样,包括多叶和无叶情况。细NO的测量的沉积速度3 -颗粒显著(p  <0.05)比细的SO较大4个2-颗粒和类似的HNO的3,而不管多叶和无叶期间。细NO的更大的沉积速度3 -引起的NH的平衡移位的颗粒4 NO 3被发现与以前在同一地点进行的测量相似。HNO的测量的沉积速度3是低的,并与那些细NO的包括许多发射箱子3 -颗粒。较低的HNO 3沉积速度与NH 4 NO 3向气相的平衡转移有关,导致HNO 3的沉积和表观排放受到抑制,特别是在无叶期。HNO 3的排放可能是由于表面附近的HNO 3浓度高,这归因于无叶冠层的少量去除。湍流增强了HNO的向上和向下通量3。这些结果将有助于更好地了解大气中氮化合物的动力学,并准确评估氮的沉积。

更新日期:2021-05-11
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