An assessment of the ability of three-dimensional air quality models with current thermodynamic equilibrium models to predict aerosol NO-3 : Particulate matter supersites
An assessment of the ability of three-dimensional air quality models with current thermodynamic equilibrium models to predict aerosol NO-3 : Particulate matter supersites
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使用当前热力学平衡模型评估三维空气质量模型预测气溶胶 NO-3 的能力：颗粒物超级位点
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发表时间：
2005
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通讯作者：
W. Robarge
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作者：
Shaocai Yu;R. Dennis;S. Roselle;A. Nenes;J. Walker;B. Eder;K. Schere;Jenise L. Swall;W. Robarge
使用两个热力学平衡模型 ISORROPIA 和气溶胶无机物模型 (AIM) 以及三个数据集研究总硝酸盐 (TNO 3 ) 和总铵 (TNH 4 ) 在气相和气溶胶相之间的分配：来自 1999 年亚特兰大超级站点实验（夏季案例）和 2002 年匹兹堡空气质量研究 (PAQS) 超级站点实验（冬季案例）的高时间分辨率测量数据，以及1999 年北卡罗来纳州克林顿基地的 12 小时测量数据。在亚特兰大基地，两个模型都以 1.5 倍的倍数再现了大部分观测到的气溶胶 NH + 4 和 HNO 3 (NH + 4 : >94% 和 HNO 3 : >86%)，而两个模型都没有再现大部分观测到的气溶胶 NO - 3 和 NH 3 (NO - 3 : <48% 和 NH) 3：<51%），在 2 倍以内。在匹兹堡站点，两个模型在 2 倍以内重现了超过 76% 的观测到的 NO - 3。在克林顿站点，两个模型在气溶胶 NO - 3 上的表现略好于亚特兰大站点（47-58%，在 1.5 倍以内），但比匹兹堡站点差。具有高斯随机误差的热力学模型的敏感性测试表明，在许多情况下，SO 2- 4 和TNH 4 的测量误差可以解释平衡模型预测与TNO 3 分配观测之间的大部分差异。将三维 (3-D) 社区多尺度空气质量 (CMAQ) 模型的预测与美国大陆的观测结果进行比较表明，NO - 3 、HNO 3 、NH + 4 和 NH 3 的 3-D 模型的性能很大程度上取决于 TNO 3 、TNH 4 和 SO 2- 4 的性能。测试表明，与 3-D 模型的 SO 2- 4 和 TNH 4 预测相关的误差可能导致热力学模型计算在夏季和冬季情况下分别仅在 2 倍内复制基本情况 NO - 3 的 47% 和 60%。结果发现，TNH 4 的误差比SO 2- 4 的误差对NO-3 的预测更为严重。
The partitioning of total nitrate (TNO 3 ) and total ammonium (TNH 4 ) between gas and aerosol phases is studied with two thermodynamic equilibrium models, ISORROPIA and the aerosol inorganics model (AIM), and three data sets: high time resolution measurement data from the 1999 Atlanta Supersite Experiment (summer case) and the 2002 Pittsburgh Air Quality Study (PAQS) Supersite Experiment (winter case), and 12-hour measurement data from the Clinton site, North Carolina, in 1999. At the Atlanta site, both models reproduced a large percentage of the observed aerosol NH + 4 and HNO 3 (NH + 4 : >94% and HNO 3 : >86%) within a factor of 1.5, whereas neither model reproduced a majority of observed aerosol NO - 3 and NH 3 (NO - 3 : <48% and NH 3 : <51%) within a factor of 2. At the Pittsburgh site, both models reproduced more than 76% of observed NO - 3 within a factor of 2. At the Clinton site, both models performed a little better on aerosol NO - 3 (47-58% within a factor of 1.5) than at the Atlanta site but worse than at the Pittsburgh site. Sensitivity test of thermodynamic models with Gaussian random errors indicates that in many cases, measurement errors in SO 2- 4 and TNH 4 can explain a major fraction of the discrepancies between the equilibrium model predictions and observations in partitioning of TNO 3 . Comparison of predictions of the three-dimensional (3-D) Community Multiscale Air Quality (CMAQ) model with the observations over the continental United States indicates that the performance of the 3-D model for NO - 3 , HNO 3 , NH + 4 , and NH 3 strongly depends on its performance for TNO 3 , TNH 4 , and SO 2- 4 . Tests show that errors associated with SO 2- 4 and TNH 4 predictions of the 3-D model can result in the thermodynamic model calculation replicating only 47% and 60% of base case NO - 3 within a factor of 2 for summer and winter cases, respectively. It was found that errors in TNH 4 are more critical than errors in SO 2- 4 to prediction of NO - 3 .