Nonlinear response of ozone to emissions: Source apportionment and sensitivity analysis
Nonlinear response of ozone to emissions: Source apportionment and sensitivity analysis
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DOI：
10.1021/es048664m
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发表时间：
2005-09-01
影响因子：
11.4
通讯作者：
Russell, AG
中科院分区：
文献类型：
--
作者：
Cohan, DS;Hakami, A;Russell, AG
对于二次空气污染物，前体排放可能以非线性和相互依赖的方式影响浓度。我们探讨了此类污染物之一臭氧对其前体物氮氧化物（NO、）和挥发性有机化合物排放的非线性响应。在美国东南部的高臭氧事件进行建模，应用二阶直接灵敏度方法在区域空气质量模型。在此应用时，灵敏度方法忽略了大多数气溶胶和水化学过程。列入二阶灵敏度，使准确的表征响应大扰动排放。引入一个指标来表征臭氧对各源区NOx排放的非线性响应。非线性被发现增加的吨位和排放密度的源区域，排放源的影响之间的相互作用被证明是导致源的贡献归因于一个合奏的发射器和归因于每个组件的贡献之和之间的差异。介绍了一种方法，应用这些“交叉敏感性”的相互作用，以评估不确定性的敏感性和源解析估计所产生的不确定性排放清单。对于臭氧对NO_3的响应，排放速率的低估导致总源贡献的低估，但每吨敏感性的高估。
For secondary air pollutants, precursor emissions may impact concentrations in nonlinear and interdependent manners. We explore the nonlinear responses of one such pollutant, ozone, to emissions of its precursors, nitrogen oxides (NO,,) and volatile organic compounds. Modeling is conducted for a high ozone episode in the southeastern United States, applying a second-order direct sensitivity method in a regional air quality model. As applied here, the sensitivity method neglects most aerosol and aqueous chemistry processes. Inclusion of second-order sensitivities is shown to enable accurate characterization of response to large perturbations in emissions. An index is introduced to characterize the nonlinearity of ozone response to NOx emitted from each source region. Nonlinearity is found to increase with the tonnage and emission density of the source region, Interactions among the impacts of emission sources are shown to lead to discrepancies between source contribution attributed to an ensemble of emitters and the sum of the contributions attributed to each component. A method is introduced for applying these "cross-sensitivity" interactions to assess the uncertainty of sensitivity and source apportionment estimates arising from uncertainty in an emissions inventory. For ozone response to NO,, underestimates in emission rates lead to underprediction of total source contribution but overprediction of per-ton sensitivity.