| 基于PMF和源示踪物比例法的大气羰基化合物来源解析:以南京市观测为例 |
| 摘要点击 3029 全文点击 1099 投稿时间：2020-05-21 修订日期：2020-06-28 |
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| 中文关键词 羰基化合物 来源解析 源示踪物比例法(STR) 正交矩阵因子模型(PMF) 南京 |
| 英文关键词 carbonyl compounds source apportionment source tracer ratio method (STR) positive matrix factorization model (PMF) Nanjing |
| 作者 | 单位 | E-mail | | 胡崑 | 南京信息工程大学环境科学与工程学院, 江苏省大气环境与装备技术协同创新中心, 江苏省大气环境监测与污染控制高技术研究重点实验室, 南京 210044 | hukun@nuist.edu.cn | | 王鸣 | 南京信息工程大学环境科学与工程学院, 江苏省大气环境与装备技术协同创新中心, 江苏省大气环境监测与污染控制高技术研究重点实验室, 南京 210044 | wangming@nuist.edu.cn | | 王红丽 | 上海市环境科学研究院, 国家环境保护城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 景盛翱 | 上海市环境科学研究院, 国家环境保护城市大气复合污染成因与防治重点实验室, 上海 200233 | | | 陈文泰 | 南京科略环境科技有限责任公司, 南京 211800 | | | 卢兴东 | 南京信息工程大学环境科学与工程学院, 江苏省大气环境与装备技术协同创新中心, 江苏省大气环境监测与污染控制高技术研究重点实验室, 南京 210044 | |
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| 中文摘要 |
| 大气羰基化合物在对流层大气化学中发挥着重要作用，其受到直接排放和二次生成的共同影响，来源研究面临挑战.本研究基于2017年3月在南京市开展的羰基化合物观测，分别利用源示踪物比例法（STR）和正交矩阵因子模型（PMF）对羰基化合物进行来源解析，并将二者结果进行比较，以探讨导致来源解析不确定性的因素.本研究共检测出11种羰基化合物，总体积分数范围为2.57×10-9~22.83×10-9，其中甲醛、乙醛和丙酮是主要组分，分别占羰基化合物总平均体积分数的36.8%、21.6%和18.5%.通过比较乙炔和甲苯作为示踪物时，以及第5和第10百分数作为背景体积分数时解析结果的差异，探讨了示踪物选取和背景体积分数对STR解析结果的影响.PMF解析出了交通排放源、石化化工源、涂料与溶剂使用源、二次生成及背景源和化工源这5类源.二次生成及背景源是羰基化合物最主要的来源，对甲醛、乙醛和丙酮的贡献分别为56.4%、48.2%和58.3%.STR和PMF解析结果的比较发现，STR法依赖于示踪物的选取，在VOCs来源复杂地区应用时需要进行严格评估. |
| 英文摘要 |
| 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 2.57×10-9-22.83×10-9. 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. |
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