Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, PR China; State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China.
Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, PR China.
Chemosphere. 2020 Apr;245:125554. doi: 10.1016/j.chemosphere.2019.125554. Epub 2019 Dec 10.
A recent quantitative measurement of rates of new particle formation (NPF) in urban Shanghai showed that the high rates of NPF can be largely attributed to the sulfuric acid (SA)-dimethylamine (DMA) nucleation due to relatively high DMA concentration in urban atmosphere (Yao et al., Science. 2018, 361, 278). In certain atmospheric conditions, the release of DMA is accompanied with the emission of high concentration of ammonia. As a result, the ammonia (A) may participate in SA-DMA-based NPF. However, the main sources of DMA and A can be different, thereby leading to different mechanism for the SA-DMA-A-based nucleation under different atmospheric conditions. Near industrial sources with relatively high DMA concentration of 10 molecules cm, the contribution of binary SA-DMA nucleation to cluster formation is 61% at 278 K, representing a dominant pathway for NPF. However, in the region not too close to major source of DMA emission, e.g., near agriculture farmland, the routes involving ternary SA-DMA-A nucleation make a 64% contribution at 278 K with DMA concentration of 10 molecules cm, showing that A has marked impact on the cluster formation. Under such a condition, we predict that coexisting DMA and A could be detected in the process of NPF. Moreover, at winter temperatures or at higher altitudes, our calculations suggest that the clustering of initial clusters likely involve ternary SA-DMA-A clusters rather than binary SA-DMA clusters. These new insights may be helpful to analyze and predict atmospheric-condition-dependent NFP in either urban or rural regions and/or in different season of the year.
最近对上海城市地区新粒子形成(NPF)速率的定量测量表明,由于城市大气中相对较高的 DMA 浓度,NPF 的高速率主要归因于硫酸(SA)-二甲胺(DMA)成核(Yao 等人,科学。2018, 361, 278)。在某些大气条件下,DMA 的释放伴随着高浓度氨的排放。因此,氨(A)可能会参与基于 SA-DMA 的 NPF。然而,DMA 和 A 的主要来源可能不同,因此在不同的大气条件下,基于 SA-DMA-A 的成核可能具有不同的机制。在 DMA 浓度相对较高(10 个分子/cm)的工业源附近,在 278 K 时,二元 SA-DMA 成核对团簇形成的贡献为 61%,代表 NPF 的主要途径。然而,在不太接近 DMA 排放主要源的区域,例如农业农田附近,涉及三元 SA-DMA-A 成核的途径在 278 K 时的贡献为 64%,DMA 浓度为 10 个分子/cm,表明 A 对团簇形成有明显影响。在这种情况下,我们预测在 NPF 过程中可能会检测到共存的 DMA 和 A。此外,在冬季温度或较高海拔下,我们的计算表明初始团簇的聚类可能涉及三元 SA-DMA-A 团簇而不是二元 SA-DMA 团簇。这些新的见解可能有助于分析和预测城市或农村地区以及/或一年中不同季节的大气条件依赖性 NFP。