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首页> 外文期刊>Environmental Science & Technology >Molecular Composition and Volatility of Nucleated Particles from α-Pinene Oxidation between -50 ℃ and +25 ℃
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Molecular Composition and Volatility of Nucleated Particles from α-Pinene Oxidation between -50 ℃ and +25 ℃

机译:-50℃至+25℃之间α--烯氧化的成核颗粒的分子组成和挥发性

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摘要

We use a real-time temperature-programmed desorption chemical-ionization mass spectrometer (FIGAERO-CIMS) to measure particle-phase composition and volatility of nucleated particles, studying pure alpha-pinene oxidation over a wide temperature range (-50 degrees C to +25 degrees C) in the CLOUD chamber at CERN. Highly oxygenated organic molecules are much more abundant in particles formed at higher temperatures, shifting the compounds toward higher O/C and lower intrinsic (300 K) volatility. We find that pure biogenic nucleation and growth depends only weakly on temperature. This is because the positive temperature dependence of degree of oxidation (and polarity) and the negative temperature dependence of volatility counteract each other. Unlike prior work that relied on estimated volatility, we directly measure volatility via calibrated temperature-programmed desorption. Our particle-phase measurements are consistent with gas-phase results and indicate that during new-particle formation from alpha-pinene oxidation, gas-phase chemistry directly determines the properties of materials in the condensed phase. We now have consistency between measured gas-phase product concentrations, product volatility, measured and modeled growth rates, and the particle composition over most temperatures found in the troposphere.
机译:我们使用实时程序升温解吸化学电离质谱仪(FIGAERO-CIMS)来测量颗粒相组成和有核颗粒的挥发性,研究在较宽的温度范围(-50摄氏度至+ 25摄氏度)在CERN的CLOUD室内。高氧有机分子在高温下形成的颗粒中含量更高,从而使化合物趋向于更高的O / C和更低的固有(300 K)挥发性。我们发现纯生物成核和生长仅在很小程度上取决于温度。这是因为氧化程度(和极性)的正温度依赖性和挥发性的负温度依赖性相互抵消。与先前的工作依赖于估计的挥发性不同,我们通过校准的程序升温脱附来直接测量挥发性。我们的颗粒相测量结果与气相结果一致,表明在由α-pine烯氧化形成新颗粒的过程中,气相化学性质直接决定了凝聚相中材料的性能。现在,我们在测得的气相产物浓度,产物挥发性,测得的和建模的增长率以及对流层中大多数温度下的颗粒组成之间具有一致性。

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