农田系统中典型污染物的运移转化与生态效应研究
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摘要
土壤是生态环境中污染物的主要载体,土壤污染直接关乎环境质量和人类健康。掌握污染物进入土壤后在各介质中的转化和运移规律,将有助于环境质量评价和污染防治政策的制订。目前研究主要关注污染物在单一介质或特定界面上的环境行为,缺乏关于污染物进入土壤后在各介质各界面环境行为的系统研究,尤其缺少长期的野外农田系统研究,研究成果难以为治理决策的制订提供科学的支持。本研究利用野外农田原状土柱(lysimeter)试验,在受控体系中对典型污染物(以BDE-209为代表的多溴联苯醚类污染物,以菲(phenanthrene)和萘(naphthalene)为代表的多环芳烃类污染物和以纳米氧化锌(nano-ZnO)和纳米二氧化钛(nano-TiO2)为代表的纳米颗粒类污染物)在农田系统中的运移转化和生态效应展开长期研究。在监测污染物随渗滤液的损耗及其在土壤纵向运移、污染物在植物体内的运移和转化的基础上获得土壤污染物在野外农田系统的环境归趋。并通过分析污染物长时间作用下对土壤酶活性和植物生长的影响以及污染物在生物体内的残留,评价了野外实际耕作条件下污染物的生态效应。主要研究结论如下：
1.通过4年的野外实验,获得了稻麦轮作的农田系统中BDE-209的半衰期约为12年,表明其在实际农田中具有很强的持久性；BDE-209污染4年后,其在土壤中的残留仍会影响作物生长和土壤质量,水稻地上部生物量降低8.3%,穗重降低5.2%,土壤脲酶活性被诱导,蛋白酶活性被抑制,有可能对土壤的肥力供应产生一定的影响；在土壤和植物体内均检测到BDE-209及其脱溴产物,土壤中BDE-47、BDE-153和BDE-183含量较高,植物体内低溴化合物的富集系数比母体BDE-209高,一方面低溴产物因Kow值比BDE-209低,更容易被植物吸收利用,另一方面存在植物体内脱溴反应的可能,表明BDE-209有通过食物链传递的风险；发现在稻麦轮作农田系统中BDE-209及其脱溴产物存在明显的纵向迁移现象,本实验条件下的纵向运移平均速率为1.54mg·m-2·yr-1,土壤中的BDE-209长期存在,有可能对地下水造成严重威胁。
2.比较了人工纳米颗粒nano-ZnO和nano-TiO2进入土壤环境后的短期、长期效应,发现nano-ZnO和nano-TiO2初期均会引起小麦生物量降低,对小麦产生一定的毒害作用,其机制可能是通过纳米颗粒形态引发损伤(nano-TiO2)或者通过溶解释放重金属离子产生毒害(nano-ZnO)作用；采用TEM观察到nano-TiO2颗粒可在小麦根尖细胞壁累积,并有少量进入周皮细胞；生长在nano-ZnO污染土壤中的小麦组织中Zn元素含量明显升高,但不确定是否存在纳米颗粒的形态；经过5个生长期的稻麦轮作,两种纳米颗粒污染在lysimeter中随渗滤液损失较少,Zn/Ti元素均未发现明显的纵向运移现象,表明其和土壤组分的结合作用较强,同时随着时间的延续,老化作用明显,纳米颗粒污染初期对土壤酶活性的显著影响2.5年后不再显著；经过2.5年后,nano-ZnO污染对作物生物量不再有明显影响,但nano-TiO2污染仍然促进作物生长,生物量增加。本发现对于全面评价纳米材料进入土壤环境后的生态风险具有重要的借鉴价值。
3.通过4年8个生长期的连续稻麦轮作,发现外源多环芳烃及其转化产物在lysimeter中的残留约为初始量的9.6%(萘)和17.7%(菲),其中母体化合物均约占初始量的1.3%。经过四年的老化作用,残留的PAHs仍然对土壤中植物的生长产生胁迫作用,萘和菲污染的lysimeter中地上部总生物量分别降低2.9%和3.2%；残留的多环芳烃还可能对土壤微生物生态系统产生一定的影响,残留菲对土壤中脲酶和过氧化物酶的活性仍表现显著诱导,但萘污染的残留组土壤酶活性差异并不显著。该结果表明对于多环芳烃污染的防治在关注不同化合物生态效应的同时应协同考虑其累积效应。
4.通过4年的野外lysimeter实验,研究获得了PAHs萘和菲在土壤中的纵向迁移规律和对地下水的影响。针对发现的PAHs胶体易化运移现象,开展了PAHs在不同粒径土壤颗粒上的吸附分离实验和室内土柱实验,结合14C示踪技术及多种微观观测手段,研究了不同粒径土壤胶体在不同pH和离子强度条件下的释放,基本结构特征及对菲的吸附能力、包气带胶体的释放及对菲的运移作用。结果表明：不同粒径胶体颗粒的元素组成差异明显,对菲的吸附能力差异也较明显,较小粒径(<0.45μm)土壤胶体颗粒对菲的吸附能力较强,但是较大颗粒(2-0.45μm)由于数量上的绝对优势对菲的吸附贡献最大；条件稳定不变时,碱性低离子强度条件有利于土壤胶体颗粒的释放,酸性高离子强度条件有利于菲在胶体上的吸附；离子强度、pH值和干湿交替等条件发生改变时土壤胶体的释放增加,但是对菲在土柱中的运移作用影响不一,离子强度降低和碱化(pH=7变为pH=9)有利于菲以溶解态形式释放运移,离子强度升高以及酸化(pH=7变为pH=5)有利于菲以胶体吸附形式释放运移。
本研究获得的典型污染物在野外稻麦轮作农田系统的长期环境归趋和生态效应,为定量评估污染物对土壤环境、食品安全以及地下水威胁提供了科学依据；相关成果和研究经验为进一步开展气候变化条件下污染物在地球关键区的环境行为和生态效应研究打下了坚实的基础,具有重要的潜在应用价值。
Soil is a major sink for pollutants released to the environment. In soil, pollutants could transport and transform in components and interfaces, threatening the safety of soil, creature, atmosphere and groundwater. Reactions and processes of pollutants in soil, plants, and other individual components or interfaces, stretching from tops of plants to the saturated aquifer, have been characterized to some extent. But few studies have examined behaviors of pollutants in agricultural field as a whole system, especially studies carried outdoor for long period. Performed over years in outdoor lysimeters with rice-wheat rotation planting, our studies offered a systemic insight into the fate and ecologic effect of PBDEs (BDE-209), nanomaterials (nano-ZnO and nano-TiO2) and PAHs (phenanthrene and naphthalene) in agricultural soil. Gaseous losses, leaching losses, residue in soil, vertical transport, plant uptake were all quantified. Differences in soil enzymes between blank soil and spiked soil over years aging were also assessed to evaluate their actual effects on soil quality. The main findings arethe followings:
1. BDE-209was demonstrated to be persistent with low degradation rate in field, and the half-life of BDE-209was calculated to be12years. By restraining plant biomass (by8.3%for overgroud part, by5.2%for spike), elevating the urease activity and inhibiting the protease activity, BDE-209still had influences on crop growth and soil quality after4years of spiking. BDE-209in the soil decreased mainly through leaching losses. Among the debrominated congeners (BDE-28,47,99,100,153,154,183), BDE-47, BDE-153and BDE-183contributed the highest percent in soil. BDE-209and seven lower brominated PBDEs were all detected in plants. There might be further debromination of BDE-209inside plants and low brominated congeners were more readily to be taken up by plants for lower Kow. Vertical trend of BDE-209over years showed its significant vertical migration in the soil column and its net average migration rate was calculated to be1.54mg·m-2·yr-1.
2. Ecological effects of the two naopartciles (TiO2, ZnO) were evaluated for short-term and long-term (2.5yrs). In early period, both of the nanoparticles reduced the biomass of wheat. The mechanisms of toxication caused by the two NPs differed in this study:the toxicity of the TiO2NPs might result from the presence of the NPs in cells or accumulated on the cell walls, and the phytotoxicity of ZnO NPs to wheat was due to the dissolved Zn. The TiO2nanoparticles were retained in the soil for long periods and primarily adhered to cell walls of periderm cells. Some small-sized TiO2NPs penetrated through the cell wall, which were dark particles found in cortex cells. The ZnO nanoparticles dissolved in the soil, thereby enhancing the uptake of toxic Zn by wheat. The applied NPs clearly affected the soil environment in early period, as evidenced by the changes in soil enzyme activities, but after2.5years the changes were unsignificant. After2.5years, there was no difference of crop biomass between growth in control and soil spiked with nano-ZnO, but crop growth in soil spiked with nano-TiO2was increased.
3. Four years after spiking,17.7%and9.6%of14C-chemical applied were detected in soil spiked with naphthalene and phenanthrene, respectively, and1.3%of C-chemical applied was found as parent compound. Residual concentration of PAHs in soil can not be ignored, restraining the crop growth and grain yeild. Residue of naphtalene in soil after4years has no significant effect on soil enzyme activities, but phenathrene residue still affected the soil quality by influencing enzyme activities.
4. Colloid-facilitated transport of PAHs found in lysimeter experiment was further investigated. Soil column experiments and adsorption test were carried out to investigate release of colloid and its transport of phenanthrene in vadose zone. Colloid particles of different sizes were of different elemental composition and also had different adsorption abilities of phenanthrene. Colloid particles with smaller size (<0.45μm) had stronger adsorption ability, but2-0.45μm colloid particles contributed to the most adsorption capacity due to their absolute advantage in number. Under steady conditions, alkaline and low ionic strength conditions were more in favor of the release of colloid particles, but acidic and high ionic strength conditions were more in favor of the adsorption of phenanthrene on colloid particles. Under change conditions, changers of ionic strength, pH value and alternating of drying and wetting, all promoted the release of colloid. Decrease in ionic strength and changes of pH value from7to9were in favor of the release of dissolved phenanthrene. Increase in ionic strength and changes of pH value from7to5were in favor of the release of adsorptive phenanthrene on colloid. The experiment confirmed colloid-facilited transport of phenanthrene, which was effected by changing conditions.
These results on long-term fate and ecological effects of typical contaminants in agricultutal field contributed to assessment influences of soil pollution on groundwater and food safety. Study on colloid release and its effects on contaminant transport in vadose zone provided basic data and method support for further large scale studies of colloid-facilitied transport of pollutants. Environment behaviors of typical pollutants especially emerging contaminants in earth's critical zone still need future work.
1.通过4年的野外实验,获得了稻麦轮作的农田系统中BDE-209的半衰期约为12年,表明其在实际农田中具有很强的持久性；BDE-209污染4年后,其在土壤中的残留仍会影响作物生长和土壤质量,水稻地上部生物量降低8.3%,穗重降低5.2%,土壤脲酶活性被诱导,蛋白酶活性被抑制,有可能对土壤的肥力供应产生一定的影响；在土壤和植物体内均检测到BDE-209及其脱溴产物,土壤中BDE-47、BDE-153和BDE-183含量较高,植物体内低溴化合物的富集系数比母体BDE-209高,一方面低溴产物因Kow值比BDE-209低,更容易被植物吸收利用,另一方面存在植物体内脱溴反应的可能,表明BDE-209有通过食物链传递的风险；发现在稻麦轮作农田系统中BDE-209及其脱溴产物存在明显的纵向迁移现象,本实验条件下的纵向运移平均速率为1.54mg·m-2·yr-1,土壤中的BDE-209长期存在,有可能对地下水造成严重威胁。
2.比较了人工纳米颗粒nano-ZnO和nano-TiO2进入土壤环境后的短期、长期效应,发现nano-ZnO和nano-TiO2初期均会引起小麦生物量降低,对小麦产生一定的毒害作用,其机制可能是通过纳米颗粒形态引发损伤(nano-TiO2)或者通过溶解释放重金属离子产生毒害(nano-ZnO)作用；采用TEM观察到nano-TiO2颗粒可在小麦根尖细胞壁累积,并有少量进入周皮细胞；生长在nano-ZnO污染土壤中的小麦组织中Zn元素含量明显升高,但不确定是否存在纳米颗粒的形态；经过5个生长期的稻麦轮作,两种纳米颗粒污染在lysimeter中随渗滤液损失较少,Zn/Ti元素均未发现明显的纵向运移现象,表明其和土壤组分的结合作用较强,同时随着时间的延续,老化作用明显,纳米颗粒污染初期对土壤酶活性的显著影响2.5年后不再显著；经过2.5年后,nano-ZnO污染对作物生物量不再有明显影响,但nano-TiO2污染仍然促进作物生长,生物量增加。本发现对于全面评价纳米材料进入土壤环境后的生态风险具有重要的借鉴价值。
3.通过4年8个生长期的连续稻麦轮作,发现外源多环芳烃及其转化产物在lysimeter中的残留约为初始量的9.6%(萘)和17.7%(菲),其中母体化合物均约占初始量的1.3%。经过四年的老化作用,残留的PAHs仍然对土壤中植物的生长产生胁迫作用,萘和菲污染的lysimeter中地上部总生物量分别降低2.9%和3.2%；残留的多环芳烃还可能对土壤微生物生态系统产生一定的影响,残留菲对土壤中脲酶和过氧化物酶的活性仍表现显著诱导,但萘污染的残留组土壤酶活性差异并不显著。该结果表明对于多环芳烃污染的防治在关注不同化合物生态效应的同时应协同考虑其累积效应。
4.通过4年的野外lysimeter实验,研究获得了PAHs萘和菲在土壤中的纵向迁移规律和对地下水的影响。针对发现的PAHs胶体易化运移现象,开展了PAHs在不同粒径土壤颗粒上的吸附分离实验和室内土柱实验,结合14C示踪技术及多种微观观测手段,研究了不同粒径土壤胶体在不同pH和离子强度条件下的释放,基本结构特征及对菲的吸附能力、包气带胶体的释放及对菲的运移作用。结果表明：不同粒径胶体颗粒的元素组成差异明显,对菲的吸附能力差异也较明显,较小粒径(<0.45μm)土壤胶体颗粒对菲的吸附能力较强,但是较大颗粒(2-0.45μm)由于数量上的绝对优势对菲的吸附贡献最大；条件稳定不变时,碱性低离子强度条件有利于土壤胶体颗粒的释放,酸性高离子强度条件有利于菲在胶体上的吸附；离子强度、pH值和干湿交替等条件发生改变时土壤胶体的释放增加,但是对菲在土柱中的运移作用影响不一,离子强度降低和碱化(pH=7变为pH=9)有利于菲以溶解态形式释放运移,离子强度升高以及酸化(pH=7变为pH=5)有利于菲以胶体吸附形式释放运移。
本研究获得的典型污染物在野外稻麦轮作农田系统的长期环境归趋和生态效应,为定量评估污染物对土壤环境、食品安全以及地下水威胁提供了科学依据；相关成果和研究经验为进一步开展气候变化条件下污染物在地球关键区的环境行为和生态效应研究打下了坚实的基础,具有重要的潜在应用价值。
Soil is a major sink for pollutants released to the environment. In soil, pollutants could transport and transform in components and interfaces, threatening the safety of soil, creature, atmosphere and groundwater. Reactions and processes of pollutants in soil, plants, and other individual components or interfaces, stretching from tops of plants to the saturated aquifer, have been characterized to some extent. But few studies have examined behaviors of pollutants in agricultural field as a whole system, especially studies carried outdoor for long period. Performed over years in outdoor lysimeters with rice-wheat rotation planting, our studies offered a systemic insight into the fate and ecologic effect of PBDEs (BDE-209), nanomaterials (nano-ZnO and nano-TiO2) and PAHs (phenanthrene and naphthalene) in agricultural soil. Gaseous losses, leaching losses, residue in soil, vertical transport, plant uptake were all quantified. Differences in soil enzymes between blank soil and spiked soil over years aging were also assessed to evaluate their actual effects on soil quality. The main findings arethe followings:
1. BDE-209was demonstrated to be persistent with low degradation rate in field, and the half-life of BDE-209was calculated to be12years. By restraining plant biomass (by8.3%for overgroud part, by5.2%for spike), elevating the urease activity and inhibiting the protease activity, BDE-209still had influences on crop growth and soil quality after4years of spiking. BDE-209in the soil decreased mainly through leaching losses. Among the debrominated congeners (BDE-28,47,99,100,153,154,183), BDE-47, BDE-153and BDE-183contributed the highest percent in soil. BDE-209and seven lower brominated PBDEs were all detected in plants. There might be further debromination of BDE-209inside plants and low brominated congeners were more readily to be taken up by plants for lower Kow. Vertical trend of BDE-209over years showed its significant vertical migration in the soil column and its net average migration rate was calculated to be1.54mg·m-2·yr-1.
2. Ecological effects of the two naopartciles (TiO2, ZnO) were evaluated for short-term and long-term (2.5yrs). In early period, both of the nanoparticles reduced the biomass of wheat. The mechanisms of toxication caused by the two NPs differed in this study:the toxicity of the TiO2NPs might result from the presence of the NPs in cells or accumulated on the cell walls, and the phytotoxicity of ZnO NPs to wheat was due to the dissolved Zn. The TiO2nanoparticles were retained in the soil for long periods and primarily adhered to cell walls of periderm cells. Some small-sized TiO2NPs penetrated through the cell wall, which were dark particles found in cortex cells. The ZnO nanoparticles dissolved in the soil, thereby enhancing the uptake of toxic Zn by wheat. The applied NPs clearly affected the soil environment in early period, as evidenced by the changes in soil enzyme activities, but after2.5years the changes were unsignificant. After2.5years, there was no difference of crop biomass between growth in control and soil spiked with nano-ZnO, but crop growth in soil spiked with nano-TiO2was increased.
3. Four years after spiking,17.7%and9.6%of14C-chemical applied were detected in soil spiked with naphthalene and phenanthrene, respectively, and1.3%of C-chemical applied was found as parent compound. Residual concentration of PAHs in soil can not be ignored, restraining the crop growth and grain yeild. Residue of naphtalene in soil after4years has no significant effect on soil enzyme activities, but phenathrene residue still affected the soil quality by influencing enzyme activities.
4. Colloid-facilitated transport of PAHs found in lysimeter experiment was further investigated. Soil column experiments and adsorption test were carried out to investigate release of colloid and its transport of phenanthrene in vadose zone. Colloid particles of different sizes were of different elemental composition and also had different adsorption abilities of phenanthrene. Colloid particles with smaller size (<0.45μm) had stronger adsorption ability, but2-0.45μm colloid particles contributed to the most adsorption capacity due to their absolute advantage in number. Under steady conditions, alkaline and low ionic strength conditions were more in favor of the release of colloid particles, but acidic and high ionic strength conditions were more in favor of the adsorption of phenanthrene on colloid particles. Under change conditions, changers of ionic strength, pH value and alternating of drying and wetting, all promoted the release of colloid. Decrease in ionic strength and changes of pH value from7to9were in favor of the release of dissolved phenanthrene. Increase in ionic strength and changes of pH value from7to5were in favor of the release of adsorptive phenanthrene on colloid. The experiment confirmed colloid-facilited transport of phenanthrene, which was effected by changing conditions.
These results on long-term fate and ecological effects of typical contaminants in agricultutal field contributed to assessment influences of soil pollution on groundwater and food safety. Study on colloid release and its effects on contaminant transport in vadose zone provided basic data and method support for further large scale studies of colloid-facilitied transport of pollutants. Environment behaviors of typical pollutants especially emerging contaminants in earth's critical zone still need future work.
引文
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19 Muresan, B.; Lorgeoux, C.; Gasperi J.; Moilleron. R. Fate and spatial variations of polybrominated diphenyl ethers in the deposition within a heavily urbanized area:case of Paris (France). Water Sci. Technol. WST.,2010,62,4,822-828.
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