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Distinct diurnal variation in organic aerosol hygroscopicity and its relationship with oxygenated organic aerosol

机译:有机气溶胶吸湿性的不同昼夜变异及其与含氧有机气溶胶的关系

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The hygroscopicity of organic aerosol (OA) is important for investigation of its climatic and environmental impacts. However, the hygroscopicity parameter κOA remains poorly characterized, especially in the relatively polluted environment on the North China Plain (NCP). Here we conducted simultaneous wintertime measurements of bulk aerosol chemical compositions of PM2.5 and PM1 and bulk aerosol hygroscopicity of PM10 and PM1 on the NCP using a capture-vaporizer time-of-flight aerosol chemical speciation monitor (CV-ToF-ACSM) and a humidified nephelometer system which measures the aerosol light-scattering enhancement factor f(RH). A method for calculating κOA based on f(RH) and bulk aerosol chemical-composition measurements was developed. We found that κOA varied in a wide range with significant diurnal variations. The derived κOA ranged from almost 0.0 to 0.25, with an average (±1σ) of 0.08 (±0.06) for the entire study. The derived κOA was highly correlated with f44 (fraction of m∕z?44 in OA measured by CV-ToF-ACSM), an indicator of the oxidation degree of OA (R=0.79), and the relationship can be parameterized as κOA=1.04×f44-0.02 (κOA=0.3×O:C-0.02, based on the relationship between the f44 and O∕C ratio for CV-ToF-ACSM). On average, κOA reached the minimum (0.02) in the morning near 07:30 local time (LT) and then increased rapidly, reaching the peak value of 0.16 near 14:30LT. The diurnal variations in κOA were highly and positively correlated with those of mass fractions of oxygenated OA (R=0.95), indicating that photochemical processing played a dominant role in the increase in κOA in winter on the NCP. Results in this study demonstrate the potential wide applications of a humidified nephelometer system together with aerosol composition measurements for investigating the hygroscopicity of OA in various environments and highlight that the parameterization of κOA as a function of OA aging processes needs to be considered in chemical transport models for better evaluating the impacts of OA on cloud formation, atmospheric chemistry, and radiative forcing.
机译:有机气溶胶(OA)的吸湿性对于调查其气候和环境影响是重要的。然而,吸湿性参数κOA特征差,特别是在华北平原(NCP)的相对污染的环境中。在这里,我们使用捕获 - 蒸发时间飞行时间气溶胶化学品质监测仪(CV-TOF-ACSM)和PM10和PM1和PM1和PM1的大量气溶胶吸湿性和PM1和PM1的大量气溶胶吸湿性的同时冬季冬季测量。一种潮湿的浊度计系统,测量气溶胶光散射增强因子F(RH)。开发了一种基于F(RH)和散装气溶胶化学组合物测量的κAA的计算方法。我们发现ΚOOA在宽范围内各种各样的差异变化。衍生的κOA的范围为0.0至0.25,平均(±1σ)为整个研究0.08(±0.06)。衍生的κOA与F44(通过CV-TOF-ACSM测量的OA中的M / Z·44的级分)高度相关,OA的氧化程度(r = 0.79)的指示器,并且该关系可以参数化为koa = 1.04×F44-0.02(ΚOA= 0.3×O:C-0.02,基于CV-TOF-ACSM的F44和O / C比率之间的关系)。平均而言,ΚOOA在局部时间(LT)附近的早晨达到最低(0.02),然后迅速增加,达到0.16近14:30LT的峰值。 κOA的昼夜变化与含氧OA(R = 0.95)的质量级分高出相关,表明光化学加工在NCP冬季κA的增加中发挥了显着作用。该研究的结果证明了一种潮湿的浊度计系统与气溶胶组成测量的潜在广泛应用,用于研究各种环境中OA的吸湿性,并强调κOA作为OA老化过程的参数化需要在化学传输模型中考虑为了更好地评估OA对云层,大气化学和辐射强制的影响。
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