Evaluation of one-dimensional and two-dimensional volatility basis sets in simulating the aging of secondary organic aerosol with smog-chamber experiments.
Evaluation of one-dimensional and two-dimensional volatility basis sets in simulating the aging of secondary organic aerosol with smog-chamber experiments.
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DOI：
10.1021/es5048914
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发表时间：
2015-01
影响因子：
11.4
通讯作者：
Bin Zhao;Shuxiao Wang;N. Donahue;W. Chuang;Lea Hildebrandt Ruiz;N. Ng;Yangjun Wang;J. Hao
中科院分区：
文献类型：
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作者：
Bin Zhao;Shuxiao Wang;N. Donahue;W. Chuang;Lea Hildebrandt Ruiz;N. Ng;Yangjun Wang;J. Hao
我们评估了一维波动性基组 (1D-VBS) 和二维波动性基组 (2D-VBS) 在模拟由甲苯和 α-蒎烯衍生的 SOA 的老化过程中对烟雾室实验的影响。如果我们用经验室拟合模拟第一代产品，并用 1D-VBS 或 2D-VBS 模拟随后的老化化学反应，则模型大多高估了甲苯氧化实验中的 SOA 浓度。这是因为经验室拟合包括第一代氧化和老化；除此之外，模拟老化会导致重复计算初始老化效果。如果明确处理第一代氧化，则基本情况 2D-VBS 会低估甲苯氧化实验的 SOA 浓度和 O:C 增加；它通常低估了 SOA 浓度并高估了 α-蒎烯实验的 O:C 增加。通过明确处理第一代氧化，我们可以分别修改甲苯和 α-蒎烯的 2D-VBS 配置，以实现良好的模型测量一致性。然而，我们无法用相同的 2D-VBS 配置来模拟甲苯和 α-蒎烯的氧化。我们建议未来的模型应该对人为（芳香）和生物前体实现并行层，并进行更多的建模研究和实验室研究以优化每个层的“最佳猜测”参数。
We evaluate the one-dimensional volatility basis set (1D-VBS) and two-dimensional volatility basis set (2D-VBS) in simulating the aging of SOA derived from toluene and α-pinene against smog-chamber experiments. If we simulate the first-generation products with empirical chamber fits and the subsequent aging chemistry with a 1D-VBS or a 2D-VBS, the models mostly overestimate the SOA concentrations in the toluene oxidation experiments. This is because the empirical chamber fits include both first-generation oxidation and aging; simulating aging in addition to this results in double counting of the initial aging effects. If the first-generation oxidation is treated explicitly, the base-case 2D-VBS underestimates the SOA concentrations and O:C increase of the toluene oxidation experiments; it generally underestimates the SOA concentrations and overestimates the O:C increase of the α-pinene experiments. With the first-generation oxidation treated explicitly, we could modify the 2D-VBS configuration individually for toluene and α-pinene to achieve good model-measurement agreement. However, we are unable to simulate the oxidation of both toluene and α-pinene with the same 2D-VBS configuration. We suggest that future models should implement parallel layers for anthropogenic (aromatic) and biogenic precursors, and that more modeling studies and laboratory research be done to optimize the "best-guess" parameters for each layer.