江苏城市污泥中PAHs的分布特征及其堆肥对PAHs（荧蒽）环境行为的影响研究
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摘要
污泥作为城市污水处理的副产物,随着污水处理事业的发展,产生量日益巨大。在污泥处理处置的方法中,污泥经过堆肥以后再进行土地利用是最适合当前我国国情的途径之一,但污泥堆肥进入土壤以后会对土壤元素的环境行为产生影响,如重金属、有机污染物等。多环芳烃(Polycyclic Aromatic Hydrocarbons,PAHs)是指两个或两个以上的苯环按线形、角状或簇状方式稠合在一起的一类中性或非极性有机化合物。由于PAHs在环境中普遍存在、难降解、持久性强和具有较强的“三致”作用,而使其在环境中的环境化学行为备受关注。因此,土壤-污泥堆肥-有机污染物的研究有助于科学合理指导污泥堆肥的利用。本论文以污泥堆肥为原料,以荧蒽(fluoranthene,FLT)为PAH的代表,采用动态取样、室内分析、污泥堆肥、土柱淋滤和室内培养等方法,系统研究了江苏城市污泥中PAHs的含量以及分布模式;堆肥对污泥中PAHs含量的影响;污泥堆肥前后水溶性有机物的理化性质特征变化;污泥堆肥对污染土壤中FLT解吸-淋滤、以及生态毒性的影响,并对有关现象进行了机理探讨。
实验室高效液相色谱(HPLC)的分析结果表明,江苏城市污泥中普遍含有多环芳烃,在美国EPA优先控制的16种污染物中,萘是江苏城市污泥中均含有的PAHs化合物,而具有强致癌性化合物苯并(a)芘的含量相对较低,在污泥中含量一般在0-2.20mg/kg,平均含量为0.15 mg/kg,远低于我国农用污泥控制标准的3.0 mg/kg。总体而言,污泥中ΣPAHs总量在11.68-169.91mg/kg,各污泥间含量差异显著;具有致癌性的PAHs含量在1.17-41.03mg/kg,平均值为6.59mg/kg;被列入中国环境“优先污染物”的PAHs含量在4.07-59.06mg/kg之间。污泥中PAHs模式呈偏态分布特征,一般含有的7-16种PAH化合物,都是以2(或3)个苯环的化合物为主,4-6个苯环的化合物的比重都较低。但污水来源及处理工艺、污泥处理方式等因素对PAHs的含量有影响。其中消化、堆肥处理可明显降低污泥中多环芳烃的含量,并改变污泥中PAHs的分布模式。
随着污泥堆肥的进行,污泥堆肥DOM含量下降,但DOM中＞8000Da大分子组分和疏水性组分含量增加,疏水性组分与亲水性组分的比值变化从0.87增至为1.34。红外光谱和紫外光谱,以及E_4/E_6比均表明,随着堆制的进行,污泥堆肥DOM的聚合程度增加,芳构化程度加深。
通过序批实验和土柱淋滤实验发现,污泥堆肥施入土壤以后因在短期内产生的水溶性有机物(DOM)而促进污染土壤中荧蒽的解吸及淋溶,但由于在原始堆肥中含有更多的有机质而使效果更加明显。但通过提取污泥堆肥前后的DOM发现,腐熟堆肥DOM因含有较多的疏水性物质和大分子量组分而较原始堆肥DOM更易促进荧蒽的解吸与淋滤。
通过生物盆栽实验发现,荧蒽对植株的生长具有抑制作用,污泥堆肥及污泥堆肥DOM的施入可以减弱这种抑制作用。土壤中的荧蒽更易在玉米根部积累,但污泥堆肥及其DOM对玉米地上部分和根部吸收荧蒽在不同的生长期的影响有差异。随着时间的延长,土壤中荧蒽的含量逐近下降,植物的存在及外源有机物的加入均能加速土壤中荧蒽含量的减少。
水培实验结果表明,荧蒽的存在抑制了玉米的生长。玉米根部比地上部分更能累积水培液中的荧蒽,污泥堆肥DOM的加入能促进植物对荧蒽的吸收和富集,并向地上部分转运,原始污泥堆肥DOM比腐熟污泥堆肥DOM的促进效果更明显。
With the development of wastewater treatment,the total amount of municipal sludges, byproduct during wastewater treatment in municipal wastewater treatment plants,increase greatly.Among the disposal methods of sludges,land application after composting is the most suitable way according to the situation of our country.But sludges after their land application will influence the environmental behaviors of soil elements such as metals and organic contaminants.Polycyclic Aromatic Hydrocarbons(PAHs) are compounds polymerized by more than two rings(including two) with linear,homed,or fascicled arrangement.They are widely distributed in the environment,hard to be degraded.Most of them are mutagens and carcinogens,and can induce malformation of embryo.Therefore, special attention has been focused on the environmental chemical behaviors of PAHs. Studies on soil-sludge composting-organic contaminants will contribute to the reasonable utilization of sludges.In our studies,sludges composting was used as object, fluoranthene(FLT) was on behalf of PAHs,and methods included dynamic sampling,room analysis,sludges' composting,leaching of soil column,and room culture were employed. The main contents include:the concentration and the distribution of PAHs in municipal sludges in Jiangsu Province,effects of composting on the concentration of PAHs in municipal sludges,the physicochemical properties of water dissolved organic matters (DOM) in sludges before and after composting,effects of sludges composting and DOM on the desorption-leaching and eco-toxicity of FLT in polluted soil,and primary investigation of mechanism on same phenomena.
Results from HPLC analysis showed that PAHs were widely distributed in municipal sludges in Jiangsu Province.Total amount of PAHs(∑PAHs,16 PAHs in the priority contaminants of US EPA) was 11.68-169.91mg/kg,and there was significant difference in∑PAHs among slidges.The total concentration ranges of carcinogenic PAHs was 1.17 to 41.03mg/kg,and the average was 6.59mg/kg.Total amount of PAHs in the priority contaminants of EPA P.R.China was 4.07-59.06mg/kg.The distribution pattern of PAHs in sludges was nonnormal.Compounds contained two(or three) benzene ring was dominant among the 7-16 PAHs found in the sludges,and the percentage of compounds contained four to six benzene ring was low.Naphthalin was the main PAHs' compounds in municipal sludges in Jiangsu Province.The contents of BaP,a strong carcinogenic PAH,was relative low,and its total concentration was 0-2.198 mg/kg,with the average of 0.152mg/kg,which was much less than 3.0 mg/kg(the control standard of sludge land application).Factors such as wastewater source,treatment technicology,and sludge treatment had great effects on PAHs contents in sludges.The digestion and composting could obviously reduce PAHs contents,and change the distribution pattern of PAHs in sludges.
With the sludges composting,content of DOM decreased.But components with molecule weight over 8000Da and hydrophobic components increased.The ratio of hydrophobic components to hydrophilic components increased from 0.87 to 1.34.Infrared spectrum,ultraviolet spectrum and E_4/E_6 showed that with the sludges composting,the polymerization and aromatization of DOM increased.
Results of sequential batch experiments and leaching of soil column showed that the application of sludges to polluted soil would promote the desorption and leaching of FLT beecause DOM produced after the application of composting sludges in a short time.But the effect would be more obvious for the primordial composting with more organic matters. Through the experiments of DOM extraction before and after composting,we found DOM from the carrion composting was more active in the enhancing of the desorption and leaching of FLT than the primordial composting,which may cause by more hydrophobic components and high-molecule-weight components in the carrion composting.
Results of pot experiments showed that there was obvious inhibiting effect of FLT on the growth of plants,and the application of composting sludges and DOM from sludges composting could mitigate this inhibiting effect.FLT in soil would be easier to be accumulated in the roots of maize.The effects of composting sludges and DOM on the accumulation of FLT in the shoots and the roots of maize showed the growth difference. With the time going on,FLT in soil decreased,and both plants and spiked organic matters could accelerate the reduction of FLT in soil.
In the water culture experiments,we found that FLT could inhibit the growth of maize. Roots of maize could absorb and accumulate more FLT than shoots from solution.DOM from sludges composting could enhance absorption and accumulation of FLT and the transfer of FLT from roots to shoots.
实验室高效液相色谱(HPLC)的分析结果表明,江苏城市污泥中普遍含有多环芳烃,在美国EPA优先控制的16种污染物中,萘是江苏城市污泥中均含有的PAHs化合物,而具有强致癌性化合物苯并(a)芘的含量相对较低,在污泥中含量一般在0-2.20mg/kg,平均含量为0.15 mg/kg,远低于我国农用污泥控制标准的3.0 mg/kg。总体而言,污泥中ΣPAHs总量在11.68-169.91mg/kg,各污泥间含量差异显著;具有致癌性的PAHs含量在1.17-41.03mg/kg,平均值为6.59mg/kg;被列入中国环境“优先污染物”的PAHs含量在4.07-59.06mg/kg之间。污泥中PAHs模式呈偏态分布特征,一般含有的7-16种PAH化合物,都是以2(或3)个苯环的化合物为主,4-6个苯环的化合物的比重都较低。但污水来源及处理工艺、污泥处理方式等因素对PAHs的含量有影响。其中消化、堆肥处理可明显降低污泥中多环芳烃的含量,并改变污泥中PAHs的分布模式。
随着污泥堆肥的进行,污泥堆肥DOM含量下降,但DOM中＞8000Da大分子组分和疏水性组分含量增加,疏水性组分与亲水性组分的比值变化从0.87增至为1.34。红外光谱和紫外光谱,以及E_4/E_6比均表明,随着堆制的进行,污泥堆肥DOM的聚合程度增加,芳构化程度加深。
通过序批实验和土柱淋滤实验发现,污泥堆肥施入土壤以后因在短期内产生的水溶性有机物(DOM)而促进污染土壤中荧蒽的解吸及淋溶,但由于在原始堆肥中含有更多的有机质而使效果更加明显。但通过提取污泥堆肥前后的DOM发现,腐熟堆肥DOM因含有较多的疏水性物质和大分子量组分而较原始堆肥DOM更易促进荧蒽的解吸与淋滤。
通过生物盆栽实验发现,荧蒽对植株的生长具有抑制作用,污泥堆肥及污泥堆肥DOM的施入可以减弱这种抑制作用。土壤中的荧蒽更易在玉米根部积累,但污泥堆肥及其DOM对玉米地上部分和根部吸收荧蒽在不同的生长期的影响有差异。随着时间的延长,土壤中荧蒽的含量逐近下降,植物的存在及外源有机物的加入均能加速土壤中荧蒽含量的减少。
水培实验结果表明,荧蒽的存在抑制了玉米的生长。玉米根部比地上部分更能累积水培液中的荧蒽,污泥堆肥DOM的加入能促进植物对荧蒽的吸收和富集,并向地上部分转运,原始污泥堆肥DOM比腐熟污泥堆肥DOM的促进效果更明显。
With the development of wastewater treatment,the total amount of municipal sludges, byproduct during wastewater treatment in municipal wastewater treatment plants,increase greatly.Among the disposal methods of sludges,land application after composting is the most suitable way according to the situation of our country.But sludges after their land application will influence the environmental behaviors of soil elements such as metals and organic contaminants.Polycyclic Aromatic Hydrocarbons(PAHs) are compounds polymerized by more than two rings(including two) with linear,homed,or fascicled arrangement.They are widely distributed in the environment,hard to be degraded.Most of them are mutagens and carcinogens,and can induce malformation of embryo.Therefore, special attention has been focused on the environmental chemical behaviors of PAHs. Studies on soil-sludge composting-organic contaminants will contribute to the reasonable utilization of sludges.In our studies,sludges composting was used as object, fluoranthene(FLT) was on behalf of PAHs,and methods included dynamic sampling,room analysis,sludges' composting,leaching of soil column,and room culture were employed. The main contents include:the concentration and the distribution of PAHs in municipal sludges in Jiangsu Province,effects of composting on the concentration of PAHs in municipal sludges,the physicochemical properties of water dissolved organic matters (DOM) in sludges before and after composting,effects of sludges composting and DOM on the desorption-leaching and eco-toxicity of FLT in polluted soil,and primary investigation of mechanism on same phenomena.
Results from HPLC analysis showed that PAHs were widely distributed in municipal sludges in Jiangsu Province.Total amount of PAHs(∑PAHs,16 PAHs in the priority contaminants of US EPA) was 11.68-169.91mg/kg,and there was significant difference in∑PAHs among slidges.The total concentration ranges of carcinogenic PAHs was 1.17 to 41.03mg/kg,and the average was 6.59mg/kg.Total amount of PAHs in the priority contaminants of EPA P.R.China was 4.07-59.06mg/kg.The distribution pattern of PAHs in sludges was nonnormal.Compounds contained two(or three) benzene ring was dominant among the 7-16 PAHs found in the sludges,and the percentage of compounds contained four to six benzene ring was low.Naphthalin was the main PAHs' compounds in municipal sludges in Jiangsu Province.The contents of BaP,a strong carcinogenic PAH,was relative low,and its total concentration was 0-2.198 mg/kg,with the average of 0.152mg/kg,which was much less than 3.0 mg/kg(the control standard of sludge land application).Factors such as wastewater source,treatment technicology,and sludge treatment had great effects on PAHs contents in sludges.The digestion and composting could obviously reduce PAHs contents,and change the distribution pattern of PAHs in sludges.
With the sludges composting,content of DOM decreased.But components with molecule weight over 8000Da and hydrophobic components increased.The ratio of hydrophobic components to hydrophilic components increased from 0.87 to 1.34.Infrared spectrum,ultraviolet spectrum and E_4/E_6 showed that with the sludges composting,the polymerization and aromatization of DOM increased.
Results of sequential batch experiments and leaching of soil column showed that the application of sludges to polluted soil would promote the desorption and leaching of FLT beecause DOM produced after the application of composting sludges in a short time.But the effect would be more obvious for the primordial composting with more organic matters. Through the experiments of DOM extraction before and after composting,we found DOM from the carrion composting was more active in the enhancing of the desorption and leaching of FLT than the primordial composting,which may cause by more hydrophobic components and high-molecule-weight components in the carrion composting.
Results of pot experiments showed that there was obvious inhibiting effect of FLT on the growth of plants,and the application of composting sludges and DOM from sludges composting could mitigate this inhibiting effect.FLT in soil would be easier to be accumulated in the roots of maize.The effects of composting sludges and DOM on the accumulation of FLT in the shoots and the roots of maize showed the growth difference. With the time going on,FLT in soil decreased,and both plants and spiked organic matters could accelerate the reduction of FLT in soil.
In the water culture experiments,we found that FLT could inhibit the growth of maize. Roots of maize could absorb and accumulate more FLT than shoots from solution.DOM from sludges composting could enhance absorption and accumulation of FLT and the transfer of FLT from roots to shoots.
引文
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