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功能性有机酸增强硫酸-二甲胺颗粒形成:一项综合实验与理论研究

Sulfuric acid-dimethylamine particle formation enhanced by functional organic acids: an integrated experimental and theoretical study.

作者信息

Wang Chunyu, Liu Yirong, Huang Teng, Feng Yajuan, Wang Zhongquan, Lu Runqi, Jiang Shuai

机构信息

School of Information Science and Technology, University of Science and Technology of China, Hefei, Anhui, 230026, China.

School of Chemistry and Material Engineering, Chaohu University, Hefei, Anhui, 238024, China.

出版信息

Phys Chem Chem Phys. 2022 Oct 5;24(38):23540-23550. doi: 10.1039/d2cp01671k.

Abstract

Atmospheric new particle formation (NPF), which has been observed globally in clean and polluted environments, is an important source of boundary-layer aerosol particles and cloud condensation nuclei, but the fundamental mechanisms leading to multi-component aerosol formation have not been well understood. Here, we use experiments and quantum chemical calculations to better understand the involvement of carboxylic acids in initial NPF from gas phase mixtures of carboxylic acid, sulfuric acid (SA), dimethylamine, and water. A turbulent flow tube coupled to an ultrafine condensation particle counter with particle size magnifier has been set up to measure NPF. Experimental results show that pyruvic acid (PA), succinic acid (SUA), and malic acid (MA) can enhance sulfuric acid-dimethylamine nucleation in the order PA < SUA < MA with a greater enhancement observed at lower SA concentrations. Computational results indicate that the carboxylic and hydroxyl groups are related to the enhancement. This experiment-theory study shows the formation of multi-component aerosol particles and the role of the organic functional group, which may aid in understanding the role of organics in aerosol nucleation and growth in polluted areas, and help to choose organic molecules of specific structures for simulation.

摘要

大气新粒子形成(NPF)在全球清洁和污染环境中均有观测到,它是边界层气溶胶粒子和云凝结核的重要来源,但导致多组分气溶胶形成的基本机制尚未得到很好的理解。在此,我们通过实验和量子化学计算,以更好地理解羧酸在由羧酸、硫酸(SA)、二甲胺和水的气相混合物引发的初始NPF过程中的作用。我们搭建了一个与配备粒径放大仪的超细凝结核计数器相连的湍流管,用于测量NPF。实验结果表明,丙酮酸(PA)、琥珀酸(SUA)和苹果酸(MA)能够增强硫酸 - 二甲胺成核作用,增强顺序为PA < SUA < MA,在较低SA浓度下观察到更大的增强效果。计算结果表明,羧基和羟基与这种增强作用有关。这项实验 - 理论研究展示了多组分气溶胶粒子的形成以及有机官能团的作用,这可能有助于理解有机物在污染地区气溶胶成核和生长中的作用,并有助于选择特定结构的有机分子进行模拟。

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