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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Temperature-dependent Henry's law constants of atmospheric organics of biogenic origin
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Temperature-dependent Henry's law constants of atmospheric organics of biogenic origin

机译：生物成因的大气有机物的温度相关亨利定律常数

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摘要

There have been growing interests in modeling studies to understand oxidation of volatile organic compounds in the gas phase and their mass transfer to the aqueous phase for their potential roles in cloud chemistry, formation of secondary organic aerosols, and fate of atmospheric organics. Temperature-dependent Henry's law constants, key parameters in the atmospheric models to account for mass transfer, are often unavailable. In the present work, we investigated gas-liquid equilibriums of isoprene, limonene, α-pinene, and linalool using a bubble column technique. These compounds, originating from biogenic sources, were selected for their implications in atmospheric cloud chemistry and secondary organic aerosol formation. We reported Henry's law constants (K_H), first order loss rates (k), and gas phase diffusion coefficients over a range of temperatures relevant to the lower atmosphere (278-298 K) for the first time. The measurement results of K_H values for isoprene, limonene, α-pinene, and linalool at 298 K were 0.036 ± 0.003; 0.048 ± 0.004; 0.029 ± 0.004; and 21.20 ± 0.30 mol L~(-1) atm~(-1), respectively. The fraction for these compounds in stratocumulus and cumulonimbus clouds at 278 K were also estimated in this work (isoprene, 1.0 × 10~(-6), 6.8 × 10 ~(-6); limonene, 1.5 × 10~(-6), 1.0 × 10 ~(-5); α-pinene, 4.5 × 10~(-7), 3.1 × 10 ~(-6); and linalool, 6.2 × 10~(-4), 4.2 × 10 ~(-3)). Our measurements in combination with literature results indicated that noncyclic alkenes could have smaller K_H values than those of cyclic terpenes and that K_H values may increase with an increasing number of double bonds. It was also shown that estimated Henry's law constants and their temperature dependence based on model prediction can differ from experimental results considerably and that direct measurements of temperature-dependent Henry's law constants of atmospheric organics are necessary for future work.
机译：为了了解挥发性有机化合物在气相中的氧化及其在水相中的传质，在云化学，二次有机气溶胶的形成以及大气有机物中的潜在作用，人们对建模研究的兴趣日益浓厚。依赖于温度的亨利定律常数（大气模型中考虑传质的关键参数）通常不可用。在目前的工作中，我们使用鼓泡塔技术研究了异戊二烯，柠檬烯，α-pine烯和芳樟醇的气液平衡。选择这些源自生物来源的化合物是因为它们对大气云化学和二次有机气溶胶形成具有影响。我们首次报告了与较低大气层相关的温度范围（278-298 K）的亨利定律常数（K_H），一阶损耗率（k）和气相扩散系数。 298 K下异戊二烯，li烯，α-pine烯和芳樟醇的K_H值的测量结果为0.036±0.003; 0.048±0.004; 0.029±0.004;和21.20±0.30 mol L〜（-1）atm〜（-1）。这项工作还估算了在278 K时平流积云和积雨云中这些化合物的分数（异戊二烯1.0×10〜（-6），6.8×10〜（-6）、;烯1.5×10〜（-6） ，1.0×10〜（-5）;α-pine烯4.5×10〜（-7），3.1×10〜（-6）;芳樟醇，6.2×10〜（-4），4.2×10〜（- 3））。我们的测量结果与文献结果相结合表明，非环状烯烃的K_H值可能小于环状萜烯的K_H值，并且随着双键数量的增加，K_H值可能会增加。还表明，基于模型预测的估计亨利定律常数及其对温度的依赖性可能与实验结果存在很大差异，直接测量大气有机物的温度依赖性亨利定律常数对于将来的工作是必要的。

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