School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China.
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China.
Sci Total Environ. 2021 Sep 10;786:147412. doi: 10.1016/j.scitotenv.2021.147412. Epub 2021 Apr 29.
Atmospheric brown carbon and their chemical behavior potentially impacts the climate and air quality. Due to lack of researches on the atmospheric chromophores by using online experimental instrument, so using the offline EEM approaches to study their types, sources and chemical processes. In this study, PILS-EEM-TOC system (Particle into liquid sampler coupled with excitation-emission matrix and total organic carbon) was developed in order to distinguish the hourly evolutions and sources of water-soluble chromophoric organic matters in atmospheric fine particles. The results suggested that the sources of atmospheric chromophores in winter were primary combustion (~90%) and coal burning, followed by biomass burning and cooking emissions in Xi'an (Northwest China). These atmospheric chromophores decay under the combined action of solar radiation and atmospheric oxidants. Meanwhile, the secondary chromophores were mainly highly-oxygenated humic-like substance (HULIS), produced by atmospheric oxidation reactions with the highest peak in the afternoon. The partly secondary chromophores can also be generated through the Maillard-like reaction in the morning, which depends on the relative humidity of the atmosphere. These findings made a deeper understanding of the sources and transformation of atmospheric brown carbon aerosols.
大气棕色碳及其化学行为可能会影响气候和空气质量。由于缺乏利用在线实验仪器研究大气发色团的研究,因此采用离线 EEM 方法来研究它们的类型、来源和化学过程。在这项研究中,开发了 PILS-EEM-TOC 系统(颗粒进入液体采样器与激发-发射矩阵和总有机碳耦合),以区分大气细颗粒物中水溶性发色有机物质的小时演变和来源。结果表明,冬季大气发色团的来源主要是一次燃烧(~90%)和煤炭燃烧,其次是生物质燃烧和烹饪排放。这些大气发色团在太阳辐射和大气氧化剂的共同作用下衰减。同时,二次发色团主要是高度氧化的类腐殖质物质(HULIS),是大气氧化反应产生的,下午达到峰值。部分二次发色团也可以通过早晨的美拉德样反应生成,这取决于大气的相对湿度。这些发现加深了对大气棕色碳气溶胶来源和转化的理解。