Rethinking organic aerosols: Semivolatile emissions and photochemical aging

Rethinking organic aerosols: Semivolatile emissions and photochemical aging
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DOI:
10.1126/science.1133061
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发表时间:
2007-03-02
期刊:
影响因子:
56.9
通讯作者:
Pandis, Spyros N.
Pandis, Spyros N.
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Robinson, Allen L.;Donahue, Neil M.;Pandis, Spyros N.

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大多数初级有机颗粒排放物是半挥发性的;因此,它们随着大气稀释而部分蒸发,产生大量的低挥发性气相材料。实验室实验表明,柴油机排放物的光氧化迅速产生有机气溶胶,大大超过了已知的二次有机气溶胶前体的贡献。我们将这种无法解释的二次有机气溶胶的产生归因于低挥发性气相物种的氧化。对一次排放的划分和光化学处理的核算产生了一个更区域分布的气溶胶,并使模型预测与观测结果更一致。控制有机颗粒物浓度将需要对目前用于测量和管理排放的方法进行重大改变。
Most primary organic-particulate emissions are semivolatile; thus, they partially evaporate with atmospheric dilution, creating substantial amounts of low-volatility gas-phase material. Laboratory experiments show that photo-oxidation of diesel emissions rapidly generates organic aerosol, greatly exceeding the contribution from known secondary organic-aerosol precursors. We attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species. Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations. Controlling organic particulate-matter concentrations will require substantial changes in the approaches that are currently used to measure and regulate emissions.