城市生活垃圾焚烧厂周围环境介质中二恶英分布规律及健康风险评估研究
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摘要
随着社会经济的高速发展、城市规模不断扩大、城市人口持续增加和居民消费结构多样化发展,我国许多城市出现垃圾“围城”现状。城市生活垃圾无害化处理成为城市管理和环境保护的重要内容,是现代社会文明程度的重要标志,直接关系人民群众的切身利益和城市的可持续稳定发展。目前,城市生活垃圾焚烧是垃圾无害化处理的重要方法之一,具有减容、减量和能量回收等显著优点。但是生活垃圾焚烧过程中存在二次污染问题,尤其二恶英排放对周围环境影响和周围居民健康危害引起了广泛的关注。
在此背景下,本文选取我国典型垃圾焚烧厂(命名为M和L),主要针对城市垃圾焚烧厂二恶英排放对周围环境介质和居民的二恶英暴露的影响以及健康风险评估,开展了一系列基础性实验和理论研究,研究的主要内容和结论如下：
1.与研究国内外垃圾焚烧厂周边环境介质中二恶英浓度水平相比,我国5个不同省份和地区16座垃圾焚烧厂建立之前周边土壤中二恶英的背景浓度(0.32～11.40ng I-TEQ/kg),M垃圾焚烧厂建厂后周边土壤中二恶英浓度水平(0.39～5.54ng I-TEQ/kg)和L垃圾焚烧厂建厂后周边土壤中二恶英浓度水平(0.972～1.46ng I-TEQ/kg),均处于世界低位水平。根据M垃圾焚烧表层土壤、深层土壤和大气中二恶英浓度检测,结合多元回归统计、二恶英指纹特征等进行源解析,以及大气中二恶英沉降通量计算的研究结果表明：M垃圾焚烧厂周围大气中二恶英浓度和沉降通量处于世界相对较高位水平。同时,M垃圾焚烧厂周边土壤中二恶英的主要来源于近年来的焚烧源排放,而历史的二恶英沉积非常小
2.利用大气扩散模型对L和M垃圾焚烧厂二恶英排放的大气扩散特性进行研究结果：二恶英大气扩散浓度分布与二恶英排放浓度成正比,同时气象条件是影响二恶英大气扩散的主要因素之一。最恶劣气象条件为风速1.5m/s和F级大气稳定度。此时混合层高度仅为100m,烟羽高度为116m,混合层高度较低不利于污染物扩散,从而导致高的地面污染浓度。根据M和L垃圾厂二恶英排放特征和气象条件,M研究区域大部分时间处于恶劣气象条件,而L研究区域有利于二恶英大气扩散,这和大气实际检测浓度相一致。
3.研究了M垃圾焚烧厂周边土壤、蔬菜中二恶英的长期和短期暴露特征,结果表明土壤和蔬菜中二恶英指纹特征与周边大气中二恶英分布相似。利用土壤和蔬菜二恶英平衡模型解析了大气-土壤-蔬菜之间二恶英的转换关系及主要来源,其结果表明土壤中二恶英主要来源于背景浓度和大气干、湿沉降,且随着时间延长土壤中二恶英受干湿沉降越明显,特别是高氯代PCDD/Fs,同时干、湿沉降对PCDFs的贡献率大于对PCDDs的贡献率。蔬菜中二恶英的主要来源于大气中二恶英气相吸附和干、湿沉降,而土壤中二恶英转移到蔬菜中含量较小。与实际监测浓度相比,土壤模型能更好地反映实际监测浓度。
4.利用Nouwen推荐的VLIER-HUMAAN模型对两座垃圾焚烧厂周围居民的二恶英环境暴露和人体健康风险进行了评估和对比分析,结果表明：人体二恶英暴露中主要通过食物摄取,其他的暴露方式相对较少。本文中提出儿童和成人的呼吸暴露与食物摄取暴露经验公式,表明人体二恶英暴露中大气呼吸暴露与食物摄取暴露存在正线性关系。对比两座垃圾焚烧厂周围环境介质中二恶英浓度水平发现,M研究区域大气中存在较高二恶英的污染,局部超过日本大气的0.6pgI-TEQ/m3标准,高出了L研究区域大气中二恶英浓度的10倍左右。根据经验公式研究结果表明M区域居民存在着较高污染风险,而L区域居民符合WHO推荐的人体日均二恶英暴露的1-4pg I-TEQ/kg·day标准。较高浓度的二恶英排放和不利于大气扩散的气象条件是导致M研究区域存在较高的二恶英暴露风险。
总之,垃圾焚烧厂周围居民二恶英暴露主要通过食物摄取,而食物中二恶英和大气中二恶英存在关联。通过大气扩散模型,沉降模型、统计分析、土壤模型和蔬菜模型计等方法研究表明二恶英的排放特征和气象条件是影响大气中二恶英浓度主要影响因素。当垃圾焚烧厂为1.0ng I-TEQ/Nm3排放时,M垃圾焚烧厂案例说明周围环境和居民健康存在一定影响,当以0.1ng I-TEQ/Nm3时,L垃圾焚烧厂案例说明二恶英排放影响较少。通过模拟计算,0.01ng Ⅰ-TEQ/Nm3排放时,二恶英排放对周围环境的影响几乎可以忽略不计。本文研究结果与关于我国修订的《生活垃圾焚烧污染控制标准》符合,和可燃固体废弃物能源化高效清洁利用机理研究(973计划)提出的0.01ng I-TEQ/Nm3排放控制目标相一致。
With rapid economic growth, massive urbanization and increasing population, treatment and management of municipal solid waste (MSW) are one of the major contents of urban management and environmental protection, and are an important hallmark of a civilized progressive society. They relates to the very interests of the people and urban stability and sustainable development. Recently, MSW incineration (MSWI) is one of important methods for MSW treatment. MSWI has remarkable advantages of reducing mass/volume and recovering energy; however, development of MSWI industry in China faces several major challenges, including secondary pollution and location problems. Especially, impact of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) emissions from MSWIs on surrounding environment and health risk has been a topic of wide concern. In order to determine the environmental impact of PCDD/F emissions from two types of MSWIs (named M and L) on surrounding environment and health risk assessment, this dissertation launched a series of fundamental experimental and theoretical studies. The objectives of the current research involved as follows:
1) The PCDD/F baseline concentrations in the soil samples, which collected near16MSWIs prior to construction in5different areas, range from0.32-11.40ng I-TEQ/kg (dry matter). The PCDD/F concentration in soil samples surround M and L MSWI is in range of0.39-5.54ng I-TEQ/kg and0.972-1.46ng I-TEQ/kg, respectively. Comparison with worldwide PCDD/F levels, the concentrations of PCDD/Fs in most soil samples are at the lower levels for rural areas (1-5ng I-TEQ/kg), indicating low contamination of baseline soils prior to the construction of16new MSWIs and soils surrounding established two types of MWSIs.
Based on the combination of the environmental monitoring data, including PCDD/F levels in air atmosphere, surface and core soils, and modeling procedures, i.e., source apportionment (including statistical analysis and fingerprint profiles) and atmospheric deposition flux model, the results indicate that PCDD/F concentration in surrounding air atmosphere and deposition flux of M MSWI are at relative high end of the world. Preliminary study also shows that the PCDD/F contamination in this area should attribute to current waste incineration, such as open burning, MSWI etc. however; the PCDD/F contamination from historical activities is very small.
2) Air distribution models are used to determine the behavior and transport of dioxin emissions both from M and L MSWIs, indicating that airborne dioxin concentration is proportional to emission levels, and meteorological data is one of the major influencing factors of dioxin airborne dispersion. Potentially severe pollution from dioxins occurs at a wind speed of1.5m/s with atmospheric stability class F, where the mixing height is only100m and height of plume rise is only116, resulting higher ground level concentration. Based on actual dioxin emission parameters and meteorological conditions, local residents in the study area of M MSWI are exposed to severe weather conditions most of time, while the study area of L MSWI is favorable to dioxin airborne dispersion. Those results are agreed with the dioxin monitoring concentration in environmental media surrounding two MSWIs.
3) The temporal and long dioxin exposure distributions in soils and vegetables surrounding the M MSWI were investigated, indicating that the dioxin fingerprint profiles both in soil and vegetable samples are similar with that in air atmospheric samples. A soil and a plant equilibrium dioxin models were carried out to determine the dioxin transfer in air-soil-vegetable system. These results show that the background concentration is the most important pathway contributing to dioxin concentrations in soil, followed by dry and wet deposition. However, the soil contamination from pathways of dry and wet deposition increases with the time, especially for higher chlorinated PCDD/Fs as well as PCDFs higher than that for PCDDs. In addition, the vapor-phase absorption and air (including dry and wet) deposition pathways are major pathways contribution to dioxin concentrations in vegetation. In both models, the uptake by roots was not obvious. Compared with dioxin monitoring concentrations in soil and vegetables, the soil model is better to predict the levels of17dioxin congeners in soils.
4) The health risks of dioxin exposure in the vicinity of MSWI were evaluated for children and adults using the VLIER-HUMAAN model recommended by Nouwen. The results indicate that the food ingestion is the major exposure pathway. Experimental formula for dioxin exposures via inhalation and food ingestion of children and adults, respectively, were derived. Based on experimental formula, it shows a good linear correlation between inhalation and food ingestion. Comparison of dioxin concentrations in air atmosphere, the dioxin concentration in air in M area is approximately10times higher than that in L area. Dioxin contaminations in parts of M area have been exceeded the Japanese Air Quality Standard (0.6pg I-TEQ/m3). According to the health risk assessment by experimental formula, risk exposure for the residents located in M area is higher than that in L area, and risk exposure for the residents in L area is agreed with the tolerable daily intake of dioxin recommended by the World Health Organization (WHO) of1-4pg TEQ/kg·day even under severe weather conditions. High risk exposure in M area attributes to higher dioxin emission concentrations and unfavorable weather to airborne.
Overall, food ingestion is major dioxin risk exposure for local residents surrounding the MSWIs, where the food ingestion is strongly related to dioxin levels in air atmosphere. Further, combination of air dispersion and atmospheric deposition, statistic analysis, air-soil-vegetable transfer models, it also indicates that dioxin emission parameters and meteorological conditions are the major influencing factors of airborne dioxin dispersion and transfer in environment surround the MSWIs. When dioxin emission concentration of the MSWI is equal to or more than1.0ng I-TEQ/Nm3, the study of site-specific exposure scenario (M MSWI) indicates that dioxin emissions from the MSWI have certain impact on surround environment and health risk. However, according to the study of site-specific exposure scenario (L MSWI), the effect of dioxin emission from the MSWI on surrounding environmental could be ignored as the dioxin emission concentration is less than0.01ng I-TEQ/Nm3. Finally, the results in this study are consistent with a new emission guideline composed by the MEP of China, and also agreed with the aim of973programme (No.2011CB201500).
在此背景下,本文选取我国典型垃圾焚烧厂(命名为M和L),主要针对城市垃圾焚烧厂二恶英排放对周围环境介质和居民的二恶英暴露的影响以及健康风险评估,开展了一系列基础性实验和理论研究,研究的主要内容和结论如下：
1.与研究国内外垃圾焚烧厂周边环境介质中二恶英浓度水平相比,我国5个不同省份和地区16座垃圾焚烧厂建立之前周边土壤中二恶英的背景浓度(0.32～11.40ng I-TEQ/kg),M垃圾焚烧厂建厂后周边土壤中二恶英浓度水平(0.39～5.54ng I-TEQ/kg)和L垃圾焚烧厂建厂后周边土壤中二恶英浓度水平(0.972～1.46ng I-TEQ/kg),均处于世界低位水平。根据M垃圾焚烧表层土壤、深层土壤和大气中二恶英浓度检测,结合多元回归统计、二恶英指纹特征等进行源解析,以及大气中二恶英沉降通量计算的研究结果表明：M垃圾焚烧厂周围大气中二恶英浓度和沉降通量处于世界相对较高位水平。同时,M垃圾焚烧厂周边土壤中二恶英的主要来源于近年来的焚烧源排放,而历史的二恶英沉积非常小
2.利用大气扩散模型对L和M垃圾焚烧厂二恶英排放的大气扩散特性进行研究结果：二恶英大气扩散浓度分布与二恶英排放浓度成正比,同时气象条件是影响二恶英大气扩散的主要因素之一。最恶劣气象条件为风速1.5m/s和F级大气稳定度。此时混合层高度仅为100m,烟羽高度为116m,混合层高度较低不利于污染物扩散,从而导致高的地面污染浓度。根据M和L垃圾厂二恶英排放特征和气象条件,M研究区域大部分时间处于恶劣气象条件,而L研究区域有利于二恶英大气扩散,这和大气实际检测浓度相一致。
3.研究了M垃圾焚烧厂周边土壤、蔬菜中二恶英的长期和短期暴露特征,结果表明土壤和蔬菜中二恶英指纹特征与周边大气中二恶英分布相似。利用土壤和蔬菜二恶英平衡模型解析了大气-土壤-蔬菜之间二恶英的转换关系及主要来源,其结果表明土壤中二恶英主要来源于背景浓度和大气干、湿沉降,且随着时间延长土壤中二恶英受干湿沉降越明显,特别是高氯代PCDD/Fs,同时干、湿沉降对PCDFs的贡献率大于对PCDDs的贡献率。蔬菜中二恶英的主要来源于大气中二恶英气相吸附和干、湿沉降,而土壤中二恶英转移到蔬菜中含量较小。与实际监测浓度相比,土壤模型能更好地反映实际监测浓度。
4.利用Nouwen推荐的VLIER-HUMAAN模型对两座垃圾焚烧厂周围居民的二恶英环境暴露和人体健康风险进行了评估和对比分析,结果表明：人体二恶英暴露中主要通过食物摄取,其他的暴露方式相对较少。本文中提出儿童和成人的呼吸暴露与食物摄取暴露经验公式,表明人体二恶英暴露中大气呼吸暴露与食物摄取暴露存在正线性关系。对比两座垃圾焚烧厂周围环境介质中二恶英浓度水平发现,M研究区域大气中存在较高二恶英的污染,局部超过日本大气的0.6pgI-TEQ/m3标准,高出了L研究区域大气中二恶英浓度的10倍左右。根据经验公式研究结果表明M区域居民存在着较高污染风险,而L区域居民符合WHO推荐的人体日均二恶英暴露的1-4pg I-TEQ/kg·day标准。较高浓度的二恶英排放和不利于大气扩散的气象条件是导致M研究区域存在较高的二恶英暴露风险。
总之,垃圾焚烧厂周围居民二恶英暴露主要通过食物摄取,而食物中二恶英和大气中二恶英存在关联。通过大气扩散模型,沉降模型、统计分析、土壤模型和蔬菜模型计等方法研究表明二恶英的排放特征和气象条件是影响大气中二恶英浓度主要影响因素。当垃圾焚烧厂为1.0ng I-TEQ/Nm3排放时,M垃圾焚烧厂案例说明周围环境和居民健康存在一定影响,当以0.1ng I-TEQ/Nm3时,L垃圾焚烧厂案例说明二恶英排放影响较少。通过模拟计算,0.01ng Ⅰ-TEQ/Nm3排放时,二恶英排放对周围环境的影响几乎可以忽略不计。本文研究结果与关于我国修订的《生活垃圾焚烧污染控制标准》符合,和可燃固体废弃物能源化高效清洁利用机理研究(973计划)提出的0.01ng I-TEQ/Nm3排放控制目标相一致。
With rapid economic growth, massive urbanization and increasing population, treatment and management of municipal solid waste (MSW) are one of the major contents of urban management and environmental protection, and are an important hallmark of a civilized progressive society. They relates to the very interests of the people and urban stability and sustainable development. Recently, MSW incineration (MSWI) is one of important methods for MSW treatment. MSWI has remarkable advantages of reducing mass/volume and recovering energy; however, development of MSWI industry in China faces several major challenges, including secondary pollution and location problems. Especially, impact of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) emissions from MSWIs on surrounding environment and health risk has been a topic of wide concern. In order to determine the environmental impact of PCDD/F emissions from two types of MSWIs (named M and L) on surrounding environment and health risk assessment, this dissertation launched a series of fundamental experimental and theoretical studies. The objectives of the current research involved as follows:
1) The PCDD/F baseline concentrations in the soil samples, which collected near16MSWIs prior to construction in5different areas, range from0.32-11.40ng I-TEQ/kg (dry matter). The PCDD/F concentration in soil samples surround M and L MSWI is in range of0.39-5.54ng I-TEQ/kg and0.972-1.46ng I-TEQ/kg, respectively. Comparison with worldwide PCDD/F levels, the concentrations of PCDD/Fs in most soil samples are at the lower levels for rural areas (1-5ng I-TEQ/kg), indicating low contamination of baseline soils prior to the construction of16new MSWIs and soils surrounding established two types of MWSIs.
Based on the combination of the environmental monitoring data, including PCDD/F levels in air atmosphere, surface and core soils, and modeling procedures, i.e., source apportionment (including statistical analysis and fingerprint profiles) and atmospheric deposition flux model, the results indicate that PCDD/F concentration in surrounding air atmosphere and deposition flux of M MSWI are at relative high end of the world. Preliminary study also shows that the PCDD/F contamination in this area should attribute to current waste incineration, such as open burning, MSWI etc. however; the PCDD/F contamination from historical activities is very small.
2) Air distribution models are used to determine the behavior and transport of dioxin emissions both from M and L MSWIs, indicating that airborne dioxin concentration is proportional to emission levels, and meteorological data is one of the major influencing factors of dioxin airborne dispersion. Potentially severe pollution from dioxins occurs at a wind speed of1.5m/s with atmospheric stability class F, where the mixing height is only100m and height of plume rise is only116, resulting higher ground level concentration. Based on actual dioxin emission parameters and meteorological conditions, local residents in the study area of M MSWI are exposed to severe weather conditions most of time, while the study area of L MSWI is favorable to dioxin airborne dispersion. Those results are agreed with the dioxin monitoring concentration in environmental media surrounding two MSWIs.
3) The temporal and long dioxin exposure distributions in soils and vegetables surrounding the M MSWI were investigated, indicating that the dioxin fingerprint profiles both in soil and vegetable samples are similar with that in air atmospheric samples. A soil and a plant equilibrium dioxin models were carried out to determine the dioxin transfer in air-soil-vegetable system. These results show that the background concentration is the most important pathway contributing to dioxin concentrations in soil, followed by dry and wet deposition. However, the soil contamination from pathways of dry and wet deposition increases with the time, especially for higher chlorinated PCDD/Fs as well as PCDFs higher than that for PCDDs. In addition, the vapor-phase absorption and air (including dry and wet) deposition pathways are major pathways contribution to dioxin concentrations in vegetation. In both models, the uptake by roots was not obvious. Compared with dioxin monitoring concentrations in soil and vegetables, the soil model is better to predict the levels of17dioxin congeners in soils.
4) The health risks of dioxin exposure in the vicinity of MSWI were evaluated for children and adults using the VLIER-HUMAAN model recommended by Nouwen. The results indicate that the food ingestion is the major exposure pathway. Experimental formula for dioxin exposures via inhalation and food ingestion of children and adults, respectively, were derived. Based on experimental formula, it shows a good linear correlation between inhalation and food ingestion. Comparison of dioxin concentrations in air atmosphere, the dioxin concentration in air in M area is approximately10times higher than that in L area. Dioxin contaminations in parts of M area have been exceeded the Japanese Air Quality Standard (0.6pg I-TEQ/m3). According to the health risk assessment by experimental formula, risk exposure for the residents located in M area is higher than that in L area, and risk exposure for the residents in L area is agreed with the tolerable daily intake of dioxin recommended by the World Health Organization (WHO) of1-4pg TEQ/kg·day even under severe weather conditions. High risk exposure in M area attributes to higher dioxin emission concentrations and unfavorable weather to airborne.
Overall, food ingestion is major dioxin risk exposure for local residents surrounding the MSWIs, where the food ingestion is strongly related to dioxin levels in air atmosphere. Further, combination of air dispersion and atmospheric deposition, statistic analysis, air-soil-vegetable transfer models, it also indicates that dioxin emission parameters and meteorological conditions are the major influencing factors of airborne dioxin dispersion and transfer in environment surround the MSWIs. When dioxin emission concentration of the MSWI is equal to or more than1.0ng I-TEQ/Nm3, the study of site-specific exposure scenario (M MSWI) indicates that dioxin emissions from the MSWI have certain impact on surround environment and health risk. However, according to the study of site-specific exposure scenario (L MSWI), the effect of dioxin emission from the MSWI on surrounding environmental could be ignored as the dioxin emission concentration is less than0.01ng I-TEQ/Nm3. Finally, the results in this study are consistent with a new emission guideline composed by the MEP of China, and also agreed with the aim of973programme (No.2011CB201500).
引文
[1]中国人民共和国国家统计局,中国统计年鉴,中国统计出版社,北京,2003.
[2]中国人民共和国国家统计局,中国统计年鉴,中国统计出版社,北京,2004.
[3]中国人民共和国国家统计局,中国统计年鉴,中国统计出版社,北京,2005.
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