Hu Kun, Wang Ming, Wang Hong-Li, Jing Sheng-Ao, Chen Wen-Tai, Lu Xing-Dong
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, Nanjing 210044, China.
State Environmental Protection Key Laboratory of Formation and Prevention of the Urban Air Complex, Shanghai Academy of Environmental Sciences, Shanghai 200233, China.
Huan Jing Ke Xue. 2021 Jan 8;42(1):45-54. doi: 10.13227/j.hjkx.202005224.
Ambient carbonyl compounds play an important role in tropospheric atmospheric chemistry. Primary emissions and photochemical formation are both sources of carbonyls, and therefore it is challenging work to analyze their sources. In this study, carbonyl sources were apportioned using the source tracer ratio method (STR) and positive matrix factorization model (PMF) based on offline carbonyls observations at a site in Nanjing during March 2017. Eleven carbonyl compounds were detected, and their total concentrations were in the range of 2.57×10-22.83×10. Formaldehyde, acetaldehyde, and acetone were the main components, accounting for 36.8%, 21.6%, and 18.5% of the average concentration of eleven carbonyl compounds, respectively. The influences of tracer selection and background concentrations on the results of source apportionment using the STR method based on comparing the results of acetylene and toluene as tracers and the 5th and 10th percentages as background concentrations are presented. Five sources were resolved by PMF, including traffic emission, the petrochemical & chemical industry, paint & solvent use, secondary formation & background, and the chemical industry. Secondary formation & background sources were the largest contributors of carbonyl compounds, contributing 56.4%, 48.2%, and 58.3% to formaldehyde, acetaldehyde, and acetone, respectively. By comparing the carbonyl source apportionment results by STR and PMF, it was found that the STR depends on the selection of tracers. When the STR is applied in the areas with complex sources, it is difficult to use a tracer to indicate anthropogenic source emissions, and therefore it is not a suitable method for carbonyl source apportionment.
大气羰基化合物在对流层大气化学中起着重要作用。一次排放和光化学形成都是羰基的来源，因此分析它们的来源是一项具有挑战性的工作。本研究基于2017年3月南京某站点的离线羰基观测数据，采用源示踪剂比值法（STR）和正定矩阵因子分解模型（PMF）对羰基来源进行了 apportioned 。检测到11种羰基化合物，其总浓度在2.57×10 - 22.83×10范围内。甲醛、乙醛和丙酮是主要成分，分别占11种羰基化合物平均浓度的36.8%、21.6%和18.5%。通过比较以乙炔和甲苯为示踪剂以及以第5和第10百分位数为背景浓度时，展示了示踪剂选择和背景浓度对使用STR方法进行源 apportionment 结果的影响。通过PMF解析出5个来源，包括交通排放、石油化工和化学工业、涂料和溶剂使用、二次形成和背景以及化学工业。二次形成和背景来源是羰基化合物的最大贡献者，分别占甲醛、乙醛和丙酮的56.4%、48.2%和58.3%。通过比较STR和PMF对羰基源 apportionment 的结果，发现STR取决于示踪剂的选择。当STR应用于源复杂的地区时，很难用一种示踪剂来指示人为源排放，因此它不是一种适合用于羰基源 apportionment 的方法。 （注：“apportioned”此处翻译为“源解析”可能更合适，但原文未给出准确对应中文词汇，按要求保留英文）
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