Pollution Characteristics and Source Analysis of Polycyclic Aromatic Hydrocarbons in the Atmosphere of Southeast Tibet
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摘要: 为探究青藏高原东南部大气中多环芳烃（Polycyclic Aromatic Hydrocarbons，简称PAHs）的污染、源及输送特征，利用鲁朗地区（29.77°N，94.73°E）总悬浮颗粒物（Total Suspended Particles，简称TSP）和大气中的14种PAHs含量，结合同期气象环境数据进行了综合分析。结果表明，该地区TSP中PAHs和气相的PAHs质量浓度变化范围分别为0.22～5.05 ng m−3和0.83～63.75 ng m−3，平均值分别为2.13 ng m−3和11.33 ng m−3。薪柴和柴油的燃烧是污染的主要方式，汽油燃烧等其他排放为次要方式。PAHs来自本地污染和远距离传输（Long Range Transmission，简称LRT）共同的影响。本地污染在四季各个源地均不相同。冬春季本地污染大，源在东南及正南方，夏秋季受本地和外来输送共同作用，本地源在东南方且占比小，LRT占比大。LRT受西北气流、西风气流和西南气流三支气流影响，污染严重时西南气流占主导，西风气流次之，污染较轻时西风气流或西北气流占主导，西北气流所传输的污染最少。该研究结果加深了对藏东南区域PAHs变化、输送特征的认识，为该区域大气污染治理提供了理论依据。Abstract: To investigate the pollution, source, and transport characteristics of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere of the southeast of Tibetan Plateau, a comprehensive analysis was carried out using 14 different PAHs from the total suspended particulate (TSP) matter and the atmospheric gaseous state in the Lulang area (29.77°N, 94.73°E) and combined with meteorological environment data from the same period. The results show that the variation ranges of PAHs mass concentration in TSP and gas phase are 0.22–5.05 ng m−3 and 0.83–63.75 ng m−3, respectively, with average values of 2.13 ng m−3 and 11.33 ng m−3. The primary source of pollution is the combustion of firewood and diesel, while other sources of pollution include the combustion of gasoline. PAHs are emitted by both local pollution and long-range transmission (LRT). In the four seasons, local pollution varies from source to source. Local pollution is serious in the winter and spring, and the source is in the southeast and due south. Pollution in the summer and autumn is primarily caused by local and LRT sources. The primary local source is mainly in the southeast, but LRT is dominant. The northwest air flow, westerly airflow, and southwest air flow all have an impact on the LRT. When pollution is serious, the dominant airflow is southwest, while the secondary dominant airflow is westerly. When the pollution is light, the dominant airflow is westerly or northwest, and the pollution transmitted by the northwest airflow is the least. The results of this study have contributed to a better knowledge of the changes and transport characteristics of PAHs in Southeast Tibet and a theoretical basis for the control of air pollution in this region and the improvement of plateau air quality.
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图 1 2008年11月至2011年9月（a）冬季、（b）夏季颗粒物中多环芳烃（PAHs）环数分布
Figure 1. Distributions of ring numbers of PAHs (Polycyclic Aromatic Hydrocarbons) in particular phases in (a) winter and (b) summer from November 2008 to September 2011
图 3 2008年11月至2011年9月（a–d）不同季节大气中PAHs及各组分的气粒占比
Figure 3. The ratios of gaseous to particular phase PAHs and components in (a–d) four seasons from November 2008 to September 2011
图 4 2008年11月至2011年9月（a–d）不同季节粒相PAHs浓度与风速风向关系粒相
Figure 4. The relation diagrams of the concentration of PAHs in TSP with wind speed and direction in (a–d) four seasons from November 2008 to September 2011
图 6 采样点的后向12天气团轨迹及频率（a）2009年10月26日、（b）2009年8月17日、（c）2010年9月13日、（d）2009年1月15日（填色表示频率大小，计算方式为通过经纬度网格（0.125°×0.125°）的每日两条轨迹数除以轨迹总数）
Figure 6. Track and frequency of backward 12 days air mass at sampling points (a) October 26, 2009, (b) August 17, 2009, (c) September 13, 2010, (d) January 15, 2009（The color filling indicates the frequency, and the calculation method is through the longitude and latitude grid (0.125°×0.125°) divided by the total number of tracks）
表 1 2008年11月至2011年9月不同季节总悬浮颗粒物（TSP）中PAHs质量浓度和质量分数
Table 1. Mass concentration and mass fraction of PAHs in TSP (Total Suspended Particulate matter) in different seasons from November 2008 to September 2011
多环芳烃（PAHs） 春季 夏季 秋季 冬季 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 苊烯（Acel） 4.12 0.19% 3 0.22% 6.18 0.22% 4.46 0.19% 苊（Ace） 8.33 0.38% 4.94 0.37% 12.02 0.43% 9.99 0.43% 菲（Phe） 419.24 19% 367.47 27.25% 701.82 25.05% 391.57 16.73% 蒽（Ant） 106.59 4.83% 64.4 4.78% 124.09 4.43% 64.79 2.77% 荧蒽（Fla） 164.53 7.46% 151.67 11.25% 320.73 11.45% 199.57 8.53% 芘（Pyr） 254.59 11.54% 180.93 13.41% 399.82 14.27% 298.14 12.74% 苯并(a)蒽（BaA） 111.35 5.05% 64.87 4.81% 150.55 5.37% 122.57 5.24% 䓛（Chr） 261.29 11.85% 180.07 13.35% 455 16.24% 360.5 15.41% 苯并(b)荧蒽（BbF） 166.88 7.57% 69 5.12% 119.45 4.2% 139.72 5.97% 苯并(k)荧蒽（BkF） 207.56 9.41% 82.93 6.15% 153.45 5.48% 221.71 9.47% 苯并(a)芘（BaP） 160.25 7.26% 53.2 3.95% 121 4.32% 186.64 7.98% 茚并(1,2,3-cd)芘（IcdP） 130.25 5.9% 49.07 3.64% 75.55 2.7% 108.79 4.65% 二苯并(a,h)蒽（DahA） 19.88 0.9% 7.33 0.54% 13.82 0.49% 15.43 0.66% 苯并(ghi)苝（BghiP） 191 8.66% 69.53 5.16% 148 5.28% 216.14 9.24% ∑PAHs 2205.85 100% 1348.4 100% 2801.47 100% 2340.03 100% 
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多环芳烃（PAHs） 春季 夏季 秋季 冬季 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 质量浓度/pg m−3 质量分数 苊烯（Acel） 8.45 0.18% 2.36 0.03% 15.36 0.1% 53.62 1.39% 苊（Ace） 3.87 0.08% 1.65 0.02% 7 0.04% 4.28 0.11% 菲（Phe） 2343 48.57% 4404.33 61.13% 10329.23 64.17% 2019.06 52.26% 蒽（Ant） 607.44 12.59% 958.73 13.31% 2011.62 12.5% 318.28 8.24% 荧蒽（Fla） 869.25 18.02% 964.27 13.38% 1913.69 11.89% 647.06 16.75% 芘（Pyr） 686.25 14.23% 688.53 9.56% 1414.31 8.79% 591.22 15.3% 苯并(a)蒽（BaA） 51.88 1.08% 36.11 0.5% 63.92 0.4% 34 0.88% 䓛（Chr） 210.5 4.36% 127.2 1.77% 294.46 1.83% 153 3.965 苯并(b)荧蒽（BbF） 7.63 0.16% 3.12 0.04% 4.75 0.03% 3.13 0.08% 苯并(k)荧蒽（BkF） 12.13 0.25% 9.4 0.13% 15.97 0.1% 10.94 0.28% 苯并(a)芘（BaP） 11.56 0.24% 4.33 0.06% 10.99 0.07% 12.78 0.33% 茚并(1,2,3-cd)芘（IcdP） 2.75 0.06% 1 0.01% 7.6 0.05% 8.2 0.21% 二苯并(a,h)蒽（DahA） — 0 — 0 — 0 — 0 苯并(ghi)苝（BghiP） 9 0.19% 3.62 0.05% 7.57 0.05% 7.94 0.21% ∑PAHs 4823.71 100% 7204.66 100% 16096.47 100% 3863.5 100
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表 3 PAHs各单体组分间特征比及污染源
Table 3. Characteristic ratio of the PAHs monomer components and pollution sources
源 各单体质量浓度比值 Ant/(Ant+Phe) BaA/(BaA+Chr) IcdP/(IcdP+BghiP) BaP/BghiP BaP/IcdP BaA/Chr BbF/BkF 木材 0.11～0.25
（李英红等，2015）0.41～0.57
（李英红等，2015）秸秆 0.12～0.24
（李英红等，2015）0.38～0.52
（李英红等，2015）焦化厂 0.42～0.62
（李英红等，2015）柴油燃烧 0.23～0.63
（李英红等，2015）0.3～0.4
（Bourotte et al., 2005）约1.0
（Menichini et al., 1999）0.2～0.4
（Simcik et al., 1999）>0.5
（Park et al., 2002）汽油燃烧 ～0.18
（Kavouras et al., 2001）0.5～0.6
（Bourotte et al., 2005）约0.4
（Menichini et al., 1999）0.3～1.2
（Simcik et al., 1999）1.1～1.5
（Dickhut et al., 2000）冶炼 0.9～6.6
（Akyüz and Çabuk，2008）1.0～1.2
（Gschwend and Hites，1981）3.5～3.9
（Masclet et al.,1987）煤炭 0.5～0.7
（Gschwend and Hites，1981）2.5～2.9
（Masclet et al.,1987）
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表 4 鲁朗地区冷暖季各单体组分间特征比及污染源
Table 4. Characteristic ratio of the PAHs monomer components and pollution sources during cold and warm season in Lulang
各单体质量浓度比值 Ant/(Ant+Phe) BaA/(BaA+Chr) IcdP/(IcdP+BghiP) BaP/BghiP BaP/IcdP BaA/Chr BbF/BkF 粒相冷季 0.16 0.27 0.37 0.85 1.44 0.37 0.72 粒相暖季 0.15 0.25 0.36 0.81 1.36 0.34 0.77 气相冷季 0.17 0.19 0.4 1.45 2.11 0.24 0.5 气相暖季 0.17 0.19 0.51 1.34 1.30 0.24 0.31
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