| 基于天津市在线数据评估ISORROPIA-Ⅱ模式结果及气溶胶pH的影响因素 |
| 摘要点击 2126 全文点击 984 投稿时间：2019-12-26 修订日期：2020-02-20 |
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| 中文关键词 气溶胶pH ISORROPIA-Ⅱ模型 模式选择 敏感性分析 影响因素 |
| 英文关键词 aerosol pH ISORROPIA-Ⅱ model mode selection sensitivity analysis influencing factors |
| 作者 | 单位 | E-mail | | 高洁 | 南开大学环境科学与工程学院, 国家环境保护城市空气颗粒物污染防治重点实验室, 天津 300350 | jiegao1996@mail.nankai.edu.cn | | 史旭荣 | 南开大学环境科学与工程学院, 国家环境保护城市空气颗粒物污染防治重点实验室, 天津 300350
环境保护部环境规划院区域空气质量模拟与管控研究中心, 北京 100012 | | | 卫昱婷 | 南开大学环境科学与工程学院, 国家环境保护城市空气颗粒物污染防治重点实验室, 天津 300350 | | | 宋少洁 | 哈佛大学工程与应用科学学院, 马萨诸塞州坎布里奇 02138 | | | 史国良 | 南开大学环境科学与工程学院, 国家环境保护城市空气颗粒物污染防治重点实验室, 天津 300350 | nksgl@nankai.edu.cn | | 冯银厂 | 南开大学环境科学与工程学院, 国家环境保护城市空气颗粒物污染防治重点实验室, 天津 300350 | |
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| 中文摘要 |
| 气溶胶酸性与颗粒物性质及二次颗粒物暴发性增长密切相关.气溶胶pH难以直接测量，通常利用热力学模型进行计算.ISORROPIA-Ⅱ是常用热力学模型之一，包括不同的模式和气溶胶状态（forward和reverse模式，stable和metastable状态），研究表明，选择的模式和相态不同，其计算的pH结果也会有差异.且除模式相态选择外，还存在其他因素也会对模型结果产生影响.为探讨在我国典型城市大气污染特征下，ISORROPIA-Ⅱ合适的模式选择以及模型结果的影响因素，本研究利用天津市高时间分辨率在线小时数据，对不同模式和气溶胶状态下的模拟结果进行了分析.结果表明，使用forward模式和metastable状态的pH计算结果较为理想.温度升高，pH、气溶胶水含量、半挥发性组分气溶胶相中浓度占比均降低.RH通过影响气溶胶水含量和半挥发性组分浓度影响气溶胶pH值.阳离子浓度升高均会不同程度地导致pH升高、气相中NH3浓度升高及HNO3浓度降低；而阴离子则相反.Ca2+、SO42-、NO3-和NH4+对pH影响较大；与SO42-相比，NO3-对pH影响较小；NH4+对pH的影响存在敏感区，高浓度NH4+不会导致pH持续升高.本研究可提高对ISORROPIA-Ⅱ模拟我国城市大气气溶胶pH的理解，为我国开展pH相关的二次生成机制、半挥发性组分气粒分配和污染控制措施等相关研究提供参考. |
| 英文摘要 |
| Aerosol acidity is closely related to particle properties and the explosive growth of secondary particles. Aerosol pH is difficult to measure directly but can be estimated indirectly by thermodynamic equilibrium modeling. ISORROPIA-Ⅱ is one of the most commonly used thermodynamic models and includes different modes (forward and reverse) and aerosol states (stable and metastable). Studies have shown that the calculated pH results vary with the selected mode and phase state. In addition to the selection of modes and phases, there are also other factors that influence the modeling results. In order to explore the appropriate mode and phase selection of ISORROPIA-Ⅱ as well as the factors influencing the model results under the air pollution characteristics of typical Chinese cities, the simulation results of different modes and aerosol states were analyzed by using online hourly data for Tianjin. The results showed that the pH calculations using the forward mode and metastable state were satisfactory at a higher RH. With increased temperature, the pH, aerosol water content, and concentration proportion in the aerosol phase of semi-volatile components all decreased. RH affected aerosol pH by influencing the aerosol water content and concentration of semi-volatile components. An increased cation concentration led to an increased pH and NH3 concentration but a decreased HNO3 concentration, whereas an increased anion concentration had the opposite effect. Ca2+, SO42-, NO3-, and NH4+ had a great influence on pH. Compared with SO42-, NO3- had less effect on pH. Sensitive areas exist in the influence of NH4+ on pH, and a high NH4+ concentration did not cause a continuous pH increase. This study can improve the understanding of aerosol pH simulation using ISORROPIA-Ⅱ, and provides reference for research on the pH-related secondary generation mechanism, semi-volatile component gas-particle distribution, and pollution control measures. |
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