Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, 219 Ningliu Road, Nanjing, 210044, China.
School of Environment Science and Engineering, Suzhou University of Science and Technology ShiHu Campus, 99 Xuefu Road, Suzhou, 215009, China.
Environ Pollut. 2023 Sep 1;332:122006. doi: 10.1016/j.envpol.2023.122006. Epub 2023 Jun 9.
Owing to the potential influence of light-absorbing organic carbon (OC), also termed "brown carbon" (BrC), on the planetary radiation budget, many studies have focused on its absorption in single-sized ranges of particulate matter (PM). However, the size distribution and organic tracer-based source apportionment of BrC absorption have not been extensively investigated. In this study, size-resolved PM samples were collected using multi-stage impactors from eastern Nanjing during each season in 2017. The light absorption of methanol-extractable OC at 365 nm (Abs, Mm) was determined using spectrophotometry, and a series of organic molecular markers (OMMs) was measured using a gas chromatography-mass spectrometer. Fine PM with an aerodynamic diameter <2.1 μm (PM) dominated Abs (79.8 ± 10.4%) of the total size ranges with maxima and minima in winter and summer, respectively. The distributions of Abs shifted to larger PM sizes from winter to spring and summer due to lower primary emissions and increased BrC chromophores in dust. Except for low-volatility (p* < 10 atm) polycyclic aromatic hydrocarbons (PAHs), the non-polar OMMs, including n-alkanes, PAHs, oxygenated PAHs, and steranes, showed a bimodal distribution pattern. Secondary products of biogenic precursors and biomass burning tracers presented a unimodal distribution peaking at 0.4-0.7 μm, while sugar alcohols and saccharides were enriched in coarse PM. Their seasonal variations in average concentrations reflected intense photochemical reactions in summer, more biomass burning emissions in winter, and stronger microbial activity in spring and summer. Positive matrix factorization was used for the source apportionment of Abs in fine and coarse PM samples. Biomass burning contributed an average of 53.9% to the Abs of PM extracts. The Abs of coarse PM extracts was associated with various dust-related sources where the aging processes of aerosol organics could occur.
由于光吸收有机碳(OC),也称为“棕色碳”(BrC),对行星辐射预算的潜在影响,许多研究都集中在其对单粒径范围颗粒物(PM)的吸收上。然而,BrC 吸收的粒径分布和基于有机示踪剂的源分配尚未得到广泛研究。在这项研究中,2017 年每个季节在南京东部使用多阶段撞击器收集了按粒径分级的 PM 样品。使用分光光度法测定甲醇提取物 OC 在 365nm 处的吸光度(Abs,Mm),并使用气相色谱-质谱仪测量一系列有机分子标记物(OMM)。空气动力学直径<2.1μm(PM)的细颗粒物(PM)主导了总粒径范围内的 Abs(79.8±10.4%),其最大值和最小值分别出现在冬季和夏季。由于初级排放物减少和尘埃中 BrC 发色团增加,Abs 的分布从冬季到春季和夏季向较大的 PM 粒径转移。除低挥发性(p*<10atm)多环芳烃(PAH)外,非极性 OMM,包括正构烷烃、PAH、含氧 PAH 和甾烷,呈双峰分布模式。生物前体的二次产物和生物质燃烧示踪剂呈单峰分布,峰值在 0.4-0.7μm 处,而糖醇和糖则富集在粗颗粒物中。它们的平均浓度季节变化反映了夏季强烈的光化学反应、冬季更多的生物质燃烧排放以及春季和夏季更强的微生物活性。正矩阵因子分析用于细颗粒物和粗颗粒物样品中 Abs 的源分配。生物质燃烧对 PM 提取物 Abs 的平均贡献为 53.9%。粗颗粒物提取物的 Abs 与各种与灰尘有关的来源有关,气溶胶有机物的老化过程可能在此发生。