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Observational Evidence for the Involvement of Dicarboxylic Acids in Particle Nucleation
Environmental Science & Technology Letters ( IF 10.9 ) Pub Date : 2020-05-19 , DOI: 10.1021/acs.estlett.0c00270
Xin Fang 1 , Min Hu 1, 2 , Dongjie Shang 1 , Rongzhi Tang 1 , Linlin Shi 3 , Tinja Olenius 4 , Yujue Wang 1 , Hui Wang 1 , Zijing Zhang 1 , Shiyi Chen 1 , Xuena Yu 1 , Wenfei Zhu 1 , Shengrong Lou 5 , Yan Ma 3 , Xin Li 1 , Limin Zeng 1 , Zhijun Wu 1 , Jun Zheng 3 , Song Guo 1
Affiliation  

Gaseous dicarboxylic acids (diacids) are suggested to participate in atmospheric new particle formation via bonding with sulfuric acid (SA), ammonia (NH3), amines, and other molecules. However, there is a lack of observational evidence for the involvement of diacids in particle nucleation. Comprehensive measurements were conducted at a rural site of the North China Plain in winter, and unexpectedly high nucleation rates (JOBS, 30.5–839.7 cm–3 s–1) were observed under low SA levels (0.7 × 106 to 4.4 × 106 cm–3). Neither SA-NH3 nor SA-dimethylamine (DMA) mechanisms could fully explain the JOBS. Gaseous diacid monomers and dimers and diacid-SA-DMA clusters were identified in this study. The JOBS values were enhanced by a factor of 5 to 10 as the signal intensities of diacids increased 4-fold. Products of diacid signals and SA concentrations showed a positive correlation with the JOBS (Pearson’s correlation coefficient = 0.72). Experimental evidence was found that succinic acid competes with the second SA molecule for addition to the SA·DMA cluster. The concentrations of diacids were estimated to be 1–3 orders of magnitude higher than those of SA. We propose that diacids could actively participate in particle nucleation and may dominate the initial steps under high [diacids]/[SA] ratios.

中文翻译:

二元羧酸参与颗粒成核的观察证据

气态二元羧酸(二元酸)被建议通过与硫酸(SA),氨(NH 3),胺和其他分子结合而参与大气新颗粒的形成。但是,缺乏观察到的证据表明二元酸参与了颗粒成核。冬季在华北平原的一个农村地区进行了全面的测量,在低SA水平(0.7×10 6到4.4×10 )下,观察到了出乎意料的高成核速率(J OBS,30.5–839.7 cm –3 s –1)。6厘米–3)。SA-NH 3和SA-二甲胺(DMA)的机制都不能完全解释J OBS。在这项研究中鉴定出气态二酸单体和二聚体以及二酸-SA-DMA簇。随着二酸信号强度增加4倍,J OBS值提高了5到10倍。二酸信号和SA浓度的乘积与J OBS呈正相关(Pearson相关系数= 0.72)。实验证据表明,琥珀酸与第二个SA分子竞争添加到SA·DMA簇中。据估计,二酸的浓度比SA的浓度高1-3个数量级。我们提出,二酸可积极参与颗粒成核,并可能在高[二酸] / [SA]比下主导初始步骤。
更新日期:2020-05-19
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