Hanze Cui , Yaxing Du , Hui Zhang , Mingqi Deng , Qi Zhang , Weihua Chen , Shuzhen Su , Xihua Li , Sayantan Sarkar , Liming Yang , Xuemei Wang , Shiguo Jia
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We find that H<sup>+</sup> concentration is the primary pathway for pH changes, contributing 64.2–81.3 %, followed by non-ideality, which accounts for 18.4–26.7 % and surpasses aerosol liquid water content (ALWC). Temperature affects pH mainly through H<sup>+</sup> concentration variation, while relative humidity influences pH primarily via ALWC. Among chemical components, sulfate and ammonium (NH<sub>4</sub><sup>+</sup>) impact pH through H<sup>+</sup>, while nitrate's influence is mainly driven by non-ideality. Excluding non-ideality shifts the fraction of NH<sub>4</sub><sup>+</sup> by as large as 48.5 %, underscoring the importance of considering non-ideality in gas-particle partitioning models. 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引用次数: 0
摘要
气溶胶酸度在大气过程中起着至关重要的作用,影响着环境和人类健康。然而,以往的研究并没有全面量化气象参数和化学成分影响pH变化的途径,特别是忽略了非理想性(γ - h +)的作用。在本研究中,我们研究了珠江三角洲城市地区气溶胶酸度的季节变化,并以此为例量化了各种途径的贡献。我们发现H+浓度是pH变化的主要途径,占64.2 - 81.3%,其次是非理想性,占18.4 - 26.7%,超过气溶胶液态水含量(ALWC)。温度主要通过H+浓度变化影响pH,相对湿度主要通过ALWC影响pH。化学成分中,硫酸盐和铵(NH4+)通过H+影响pH,而硝酸盐的影响主要由非理想性驱动。排除非理想状态会使NH4+的分数偏移高达48.5%,这强调了在气-颗粒分配模型中考虑非理想状态的重要性。最后,离子强度和硝酸盐组分显著影响活度系数,强调在检查气溶胶酸性过程时需要考虑非理想性。
A quantitative study on the influencing pathways of aerosol acidity: the non-neglectable role of non-ideality
Aerosol acidity plays a crucial role in atmospheric processes, impacting both environmental and human health. However, previous studies have not comprehensively quantified the pathways through which meteorological parameters and chemical components influence pH changes, particularly overlooking the role of non-ideality (γH+). In this study, we investigate the seasonal variation in aerosol acidity in an urban area of the Pearl River Delta, China, as a case to quantify the contributions of various pathways. We find that H+ concentration is the primary pathway for pH changes, contributing 64.2–81.3 %, followed by non-ideality, which accounts for 18.4–26.7 % and surpasses aerosol liquid water content (ALWC). Temperature affects pH mainly through H+ concentration variation, while relative humidity influences pH primarily via ALWC. Among chemical components, sulfate and ammonium (NH4+) impact pH through H+, while nitrate's influence is mainly driven by non-ideality. Excluding non-ideality shifts the fraction of NH4+ by as large as 48.5 %, underscoring the importance of considering non-ideality in gas-particle partitioning models. Lastly, ionic strength and nitrate fraction significantly influence the activity coefficient, highlighting the need to consider non-ideality when examining aerosol acidity processes.
期刊介绍:
Atmospheric Environment has an open access mirror journal Atmospheric Environment: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review.
Atmospheric Environment is the international journal for scientists in different disciplines related to atmospheric composition and its impacts. The journal publishes scientific articles with atmospheric relevance of emissions and depositions of gaseous and particulate compounds, chemical processes and physical effects in the atmosphere, as well as impacts of the changing atmospheric composition on human health, air quality, climate change, and ecosystems.