杭州市空气中PAHs污染源及归宿研究
摘要
多环芳烃(PAHs)是大气中广泛存在的一类持久性有机污染物，占自然界中致癌物质总量1/3以上，主要来源有石油泄漏、汽车尾气、环境烟草烟雾、燃料燃烧及烹调油烟等。空气中PAHs污染严重威胁人体健康，准确把握PAHs污染现状、主要来源及归宿为有效控制PAHs污染，保护人群健康提供科学依据。本文以杭州为例，在系统研究城市室内外环境空气中PAHs的污染现状、影响因素及职业/非职业PAHs暴露的基础上，重点研究了交通干线空气中PAHs的归宿(干、湿沉降、地表径流以及PAHs在空气和地面尘土之间的循环)。系统深入研究了城市空气中各典型PAHs污染源(汽车尾气、烹调、香烟烟雾、焦化厂)排放规律、特征及影响因素，建立一份较详细的PAHs源谱图，为多途径开展PAHs源解析工作提供必要的源信息；同时为有效削减PAHs排放提供依据。建立污染源相似度参数，并用于解析水体底泥PAHs的主要来源。论文取得了一些有价值研究成果：
(1)传统烹调方式导致厨房空气中PAHs污染十分严重。商业厨房空气中12种PAHs的平均浓度17.23μg/m~3，BaP浓度均超标，家庭厨房空气中PAHs的平均浓度为7.634μg/m~3，BaP浓度超标率为83％。
(2)空气中PAHs的主要环境行为及汇机制不同。干沉降主要去除空气中4-5环PAHs，湿沉降对3环PAHs有很好的清除作用，2环PAHs主要存在于空气中，干、湿沉降对其无明显去除作用。地表径流主要能增加水体低分子量PAHs的负担，对高分子PAHs，如BaP贡献不大。空气是2环PAHs的主要载体，大部分3环和部分4环PAHs通过直接或间接途径进入水体，尘土仍然是交通干线空气中部分4环和5环PAHs的主要贮存地。
(3)建立典型污染源(汽车尾气、烹调油烟、香烟烟雾及焦化废气)PAHs成分谱图。探明典型PAHs污染源排放特征及影响因素。烹调产生PAHs与烹调方式、油品、温度有关；煎和烤产生PAHs量远高于煮；相同油温下，不同油品产生PAHs量依次为猪油＞菜籽油＞豆油；油温与PAHs产生量有明显的相关性。机动车排放PAHs量与燃油类型及里程数有关，柴油机动车排放PAHs总量大于汽油机动车，但相对毒性较小，以2、3、4环PAHs为主(共占总量的
敏
浙江大学博士学位论文
97%)，5环队Hs的贡献近乎忽略(只有2.2%);在汽油机尾气中，四环队Hs
贡献显著，达58%，2、3、5环相对含量比较相似，分别为19%、10%、13%;
相同车型的车辆，里程数越长，PAHs排放量及毒性均增强。香烟烟雾中PAHs
总量与煤焦油含量有较好的相关性，与尼古丁无明显相关性。
(4)建立了污染源相似度参数，解析河流底泥中PAHS来源。发现钱塘江
流域、西湖和内河底泥PAHs主要来源于石油泄漏，而运河底泥中队HS主要来
源于运输船只发动机的尾气排放。
Polycyclic aromatic hydrocarbons (PAHs), a kind of POPs are ubiquitous in air, contributing more than 1/3 of the total carcinogenic chemicals, with the source of oil-leak, traffic emissions, environmental tobacco smoke, fuel-burning, cooking oil-fumes, and, so on. PAHs pollution in air emphasized threat on the whole human. And the understanding of occurrence, sources and fates for PAHs in environment is the basis of controlling POPs pollution efficiently, thus reducing personal intake and protecting human health.
In China, rapid economic development has lead to heavy air pollution, especially in major cities, although with the government effective measures.
The paper took Hangzhou as a case, firstly had a comprehensive investigation into PAHs pollution in indoor and outdoor air with occupational and non-occupational PAHs intakes through breath. Then fate for PAHs in arterial air including dry, wet deposition, runoff and exchange of PAHs between air and road dust was emphasized. Deep-insight into PAHs production, characteristics in discharges and affecting factors were achieved for the dominant PAHs sources, such as traffic discharges, cooking practice, tobacco smoke and coke plant, consequently to determine the first PAHs sources fingerprints, providing detailed source information for source analysis. At the same time, it was also helpful to cut PAHs production from sources. A new parametre was established to conduct source analysis for Sediment. The main conclusions were below:
(1) Conventional cooking practise have leaded to heavy PAHs pollution in kitchens air. Average PAHs pollution in commercial kitchens air were 17.23 ng/m3 with BaP all exceeded the national air standard. Residential kitchens presented an mean PAHs concentration of 7.634 ng/m3 and 83% BaP exceeded the limitation.
(2) Fate of PAHs in air was discussed with the result shown, dry deposit mostly cleaned 4-5 ring PAHs, while wet deposit emphasized on 3 ring PAHs. Runoff had a larger contribution to low-molecular-weight PAHs in waterbody than high-molecular-weight PAHs. Air was the chief reserve for 2-ring PAHs, and 3-4 ring PAHs in air may entered waterbody through many routes. Road dust was home for 4-5 ring PAHs in air.
(3) PAHs fingerprints for typical sources were achieved. Characteristics and
determinate factors of PAHs discharge from typical sources was investigated. PAHs in oil fume were dominated by cooking practise, oil type and temperature. Frying and roasting produced much more PAHs than boiling. In the studied three edible oil, lard oil produce least PAHs followed by soybean oil and seed oil with good relation to oil temperature. PAHs in traffic emissions were in good relation to oil consumed, mileage. Diesel engine emit more PAHs of less toxic, compared to gasoline engine. 2-4 ring PAHs is predominant in diesel engine emission, accounting for 97% of the total PAHs. In gasoline engine discharges, 4-ring PAHs were the most predominant, having 58% contributions. 2-3 ring and 5 ring PAHs accounting for 19% 10% 13%, respectively for total PAHs. Vehicle of longer mileages discharged more toxic PAHs. PAHs in tobacco smoke were in good relation to tar content, having nothing to do with nicotin content.
(4) A new parameter was introduced to source analysis for PAHs in sediment, with the result showed that, PAHs in sediment from Qiantang River, West Lake and Inland river mainly came form oil-leak, and PAHs in canal mostly came from ship-engine discharges.
(1)传统烹调方式导致厨房空气中PAHs污染十分严重。商业厨房空气中12种PAHs的平均浓度17.23μg/m~3，BaP浓度均超标，家庭厨房空气中PAHs的平均浓度为7.634μg/m~3，BaP浓度超标率为83％。
(2)空气中PAHs的主要环境行为及汇机制不同。干沉降主要去除空气中4-5环PAHs，湿沉降对3环PAHs有很好的清除作用，2环PAHs主要存在于空气中，干、湿沉降对其无明显去除作用。地表径流主要能增加水体低分子量PAHs的负担，对高分子PAHs，如BaP贡献不大。空气是2环PAHs的主要载体，大部分3环和部分4环PAHs通过直接或间接途径进入水体，尘土仍然是交通干线空气中部分4环和5环PAHs的主要贮存地。
(3)建立典型污染源(汽车尾气、烹调油烟、香烟烟雾及焦化废气)PAHs成分谱图。探明典型PAHs污染源排放特征及影响因素。烹调产生PAHs与烹调方式、油品、温度有关；煎和烤产生PAHs量远高于煮；相同油温下，不同油品产生PAHs量依次为猪油＞菜籽油＞豆油；油温与PAHs产生量有明显的相关性。机动车排放PAHs量与燃油类型及里程数有关，柴油机动车排放PAHs总量大于汽油机动车，但相对毒性较小，以2、3、4环PAHs为主(共占总量的
敏
浙江大学博士学位论文
97%)，5环队Hs的贡献近乎忽略(只有2.2%);在汽油机尾气中，四环队Hs
贡献显著，达58%，2、3、5环相对含量比较相似，分别为19%、10%、13%;
相同车型的车辆，里程数越长，PAHs排放量及毒性均增强。香烟烟雾中PAHs
总量与煤焦油含量有较好的相关性，与尼古丁无明显相关性。
(4)建立了污染源相似度参数，解析河流底泥中PAHS来源。发现钱塘江
流域、西湖和内河底泥PAHs主要来源于石油泄漏，而运河底泥中队HS主要来
源于运输船只发动机的尾气排放。
Polycyclic aromatic hydrocarbons (PAHs), a kind of POPs are ubiquitous in air, contributing more than 1/3 of the total carcinogenic chemicals, with the source of oil-leak, traffic emissions, environmental tobacco smoke, fuel-burning, cooking oil-fumes, and, so on. PAHs pollution in air emphasized threat on the whole human. And the understanding of occurrence, sources and fates for PAHs in environment is the basis of controlling POPs pollution efficiently, thus reducing personal intake and protecting human health.
In China, rapid economic development has lead to heavy air pollution, especially in major cities, although with the government effective measures.
The paper took Hangzhou as a case, firstly had a comprehensive investigation into PAHs pollution in indoor and outdoor air with occupational and non-occupational PAHs intakes through breath. Then fate for PAHs in arterial air including dry, wet deposition, runoff and exchange of PAHs between air and road dust was emphasized. Deep-insight into PAHs production, characteristics in discharges and affecting factors were achieved for the dominant PAHs sources, such as traffic discharges, cooking practice, tobacco smoke and coke plant, consequently to determine the first PAHs sources fingerprints, providing detailed source information for source analysis. At the same time, it was also helpful to cut PAHs production from sources. A new parametre was established to conduct source analysis for Sediment. The main conclusions were below:
(1) Conventional cooking practise have leaded to heavy PAHs pollution in kitchens air. Average PAHs pollution in commercial kitchens air were 17.23 ng/m3 with BaP all exceeded the national air standard. Residential kitchens presented an mean PAHs concentration of 7.634 ng/m3 and 83% BaP exceeded the limitation.
(2) Fate of PAHs in air was discussed with the result shown, dry deposit mostly cleaned 4-5 ring PAHs, while wet deposit emphasized on 3 ring PAHs. Runoff had a larger contribution to low-molecular-weight PAHs in waterbody than high-molecular-weight PAHs. Air was the chief reserve for 2-ring PAHs, and 3-4 ring PAHs in air may entered waterbody through many routes. Road dust was home for 4-5 ring PAHs in air.
(3) PAHs fingerprints for typical sources were achieved. Characteristics and
determinate factors of PAHs discharge from typical sources was investigated. PAHs in oil fume were dominated by cooking practise, oil type and temperature. Frying and roasting produced much more PAHs than boiling. In the studied three edible oil, lard oil produce least PAHs followed by soybean oil and seed oil with good relation to oil temperature. PAHs in traffic emissions were in good relation to oil consumed, mileage. Diesel engine emit more PAHs of less toxic, compared to gasoline engine. 2-4 ring PAHs is predominant in diesel engine emission, accounting for 97% of the total PAHs. In gasoline engine discharges, 4-ring PAHs were the most predominant, having 58% contributions. 2-3 ring and 5 ring PAHs accounting for 19% 10% 13%, respectively for total PAHs. Vehicle of longer mileages discharged more toxic PAHs. PAHs in tobacco smoke were in good relation to tar content, having nothing to do with nicotin content.
(4) A new parameter was introduced to source analysis for PAHs in sediment, with the result showed that, PAHs in sediment from Qiantang River, West Lake and Inland river mainly came form oil-leak, and PAHs in canal mostly came from ship-engine discharges.
引文
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