Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20742, United States.
J Phys Chem A. 2023 May 4;127(17):3873-3882. doi: 10.1021/acs.jpca.2c08585. Epub 2023 Apr 20.
Black carbon (BC) is an aerosol that is released into the atmosphere due to the incomplete burning of biomass and can affect the climate directly or indirectly. BC commonly mixes with other primary or secondary aerosols to undergo aging, thereby changing its radiative properties and cloud condensation nuclei (CCN) activity. The composition of aged BC species in the atmosphere is difficult to measure with high confidence, so their associated CCN activity can be uncertain. In this work, the CCN activity analysis of BC was performed using laboratory measurements of proxy aged BC species. Vulcan XC72R carbon black was used as the representative of BC, and three structural isomers of benzenedicarboxylic acid─phthalic acid (PTA), isophthalic acid (IPTA), and terephthalic acid (TPTA)─were mixed with BC to generate three different proxies of aged BC species. Most studies related to CCN activity analysis of BC aerosols use the traditional Köhler theory or an adsorption theory (such as the Frenkel-Halsey-Hill adsorption theory). PTA, IPTA, and TPTA fall in the sparingly water-soluble range and therefore do not fully obey either of the aforementioned theories. Consequently, a novel hybrid activity model (HAM) was used for the CCN activity analysis of the BC mixtures studied in this work. HAM combines the features of adsorption theory via the adsorption isotherm with the features of Köhler theory by incorporating solubility partitioning. The results in this work showed that HAM improves the representation of CCN activity of pure and mixed BC aerosol species with high certainty, evident from generally better goodness of fit, > 0.9. This work implies that the hygroscopicity parameterization based on HAM captures the size-dependent variability in the CCN activity of the pure and aged BC species.
黑碳(BC)是由于生物质不完全燃烧而释放到大气中的气溶胶,它可以直接或间接影响气候。BC 通常与其他一次或二次气溶胶混合,经历老化,从而改变其辐射性质和云凝结核(CCN)活性。大气中老化 BC 物种的组成很难用高置信度测量,因此它们相关的 CCN 活性可能不确定。在这项工作中,使用实验室测量的替代老化 BC 物种来进行 BC 的 CCN 活性分析。Vulcan XC72R 炭黑被用作 BC 的代表,苯二甲酸(PTA)、间苯二甲酸(IPTA)和对苯二甲酸(TPTA)的三种结构异构体与 BC 混合,生成三种不同的老化 BC 物种的代表物。大多数与 BC 气溶胶 CCN 活性分析相关的研究使用传统的 Köhler 理论或吸附理论(如 Frenkel-Halsey-Hill 吸附理论)。PTA、IPTA 和 TPTA 属于难溶范围,因此不完全服从上述任何一种理论。因此,对于本工作研究的 BC 混合物的 CCN 活性分析,采用了一种新的混合活性模型(HAM)。HAM 通过吸附等温线将吸附理论的特征与溶解度分配相结合,纳入了 Köhler 理论的特征。本工作的结果表明,HAM 显著提高了纯和混合 BC 气溶胶物种 CCN 活性的代表性,拟合优度 >0.9,具有较高的可信度。这项工作表明,基于 HAM 的吸湿性参数化可以捕捉到纯和老化 BC 物种的 CCN 活性的尺寸依赖性变化。