稻田土壤重金属污染和稻米Cd安全分析及控制技术探讨
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摘要
土壤是陆地生态系统的重要支撑基础,又是地球表层环境的重要组成部分。在维持农作物生产的同时,农业土壤环境污染及其食物安全风险问题是当今农业可持续发展的重大挑战之一。南方稻田重金属污染较为普遍,特别是太湖地区、珠江三角洲地区和江西湖南红壤丘陵地区的土壤重金属污染分布及其食物安全风险评价已有多方面的研究报道。本课题组关于太湖地区重金属(特别是Cd和Zn)的土壤污染特征及农产品重金属积累以及食物安全风险已经进行了一系列的分析研究,但对重金属污染积累的团聚体组成变化及带来的重金属土壤团聚体分配的变化,不同稻区稻米重金属积累差异与稻田土壤性质的关联性等还未有系统研究探讨。污染稻田稻米重金属积累的抑制和控制技术也还未有可靠技术。
因此,本文基于已有认识,首先研究了重金属污染下稻田土壤团聚体组成变化,分析污染下土壤团聚体形成及重金属的土壤颗粒粒径分配变化,探讨重金属污染对土壤生物物理过程的影响；其次,采集南方不同稻区稻米样品,分析Cd、Zn含量,探讨与稻区土壤类型及其土壤性质特征的关系,最后从影响稻区稻米重金属水平的土壤因素-土壤酸度着手,探讨通过施用改良剂调节土壤Cd活性而降低稻米Cd积累的技术。获得结果如下：
1.本文采集已报道严重污染的水稻土和未明显污染的同种水田土壤表土样品,分析不同粒径土壤团聚体颗粒组的质量组成和Pb、Cd、Hg、As等重金属元素的含量,讨论重金属污染下土壤团聚体组成和重金属团聚体分配的变化。在重金属污染下,土壤砂粒级团聚体减少,而较细粒径团聚体相对增多；尽管重金属含量随粒径变化的趋势与先前研究认识一致,即在<0.002mm和2-0.2mm粒径的颗粒组中富集,但污染下重金属元素更多地赋存于粉砂组和黏粒组团聚体。因此,重金属污染可能减弱了较大土壤团聚体形成作用,导致细粒径团聚体的相对增多,从而明显提高重金属元素在易移动的粉砂和黏粒组团聚体的分配,这可能进一步加剧污染农田重金属的水迁移和大气颗粒物迁移的风险。
2.在江西、湖南、安徽和广东等南方典型水稻产区的农产品市场和农户随机采取大米样品共70份,分别测定样品中Cd、Zn和Se的含量,并分析不同产地大米的含量差异及其与产区主要土壤特征的关系。结果表明,70%以上的供试样品Cd含量超出国家食品卫生标准值(0.2mg·kg-1),且Cd/Zn(质量比)超出美国学者建议的0.015临界值。不同产地大米样本间所分析元素的含量及Cd/Zn均呈污染产地>酸性水稻土产地>中性水稻土产地,且以Cd和Se含量的差异幅度较大,Zn较小。说明土壤酸度及Cd有效性是影响供试大米Cd含量的主要因素。因而,土壤-水稻系统中Cd迁移与籽粒积累取决于人为污染和土壤的化学性质的共同作用。分析表明所有供试产地的大米样本对于农民就地消费来说均存在不同程度的潜在Cd暴露风险,以污染土壤产地区和酸性红壤性水稻土产地为严重。
3.根据前述结果,针对土壤酸度对稻米Cd积累的重要影响,并考虑到Cd-Zn拮抗关系和沉淀钝化作用,采用田间定位试验,探讨了不同用量的钙镁磷肥及叶面喷施锌肥(ZnSO4·7H20)等处理对降低污染稻田水稻籽粒Cd含量的影响。试验表明,不同肥料调节剂处理没有显著提高水稻产量,但籽粒Cd含量有不同程度降低。分析表明,磷肥处理提高了土壤的pH值,且随用量而增高,而土壤中有效态Cd含量相应显著降低。推测主要是由于土壤pH升高而降低了土壤Cd活性。不过,叶面喷施锌肥并未明显提高土壤pH值,但显著降低土壤有效态Cd含量,看来淹水下形成难溶性CdS而钝化了土壤Cd。施用磷肥调节剂可以通过调控土壤酸度而达到钝化稻田土壤Cd从而抑制水稻籽粒中Cd积累的效果。但是,在严重污染稻田中,这些用量尚不能有效控制稻米Cd的安全。建议严重重金属污染的土壤改种其它非Cd强积累作物。
本文的研究说明,稻田土壤污染可能影响土壤的物理性质,可能带来对土壤中各种过程的进一步影响；同时,稻田土壤污染对食物安全的影响可能受污染物数量和土壤性质的共同影响,土壤酸度差异可能是产地区域稻米Cd分异的主要因素,因而从土壤酸度调节和控制出发研究稻米重金属污染控制技术是一个今后需要努力的方向。
Soils are the physical support for the terrestrial ecosystem and also the most important component of the earth surface environment. Soil pollution and its health risks via food consumption for human is one of the great challenges for the sustainable agriculture together with the need for increasing soil productivity. Soil pollution, however, is very extensive in South China rice area, especially from the Tai Lake region, Pearl River delta region and red earth region of Jiangxi and Hunan provinces. Many studies on soil pollution of heavy metals such as Pb, Cd, As in rice paddies and the exposure risks by dietary intake have been reported. Among these, a number of studies have been conducted at Institute of Resources, Ecosystem and Environment of Agriculture (IREEA) on soil distribution, accumulation in rice grains and evaluation of food exposure risks from the Tai Lake region, Jiangsu. Whereas, the effect of heavy metals on composition of soil aggregates of different size frcationss, and thus, the distribution pattern of these polluted metals in size fractions has not yet been examed. In addition, the relationship of heavy metal concentration in rice grains with the soil properties where the rice were grown has not been elucidated. And at last, there have not yet been feasible measures for depressing the heavy metal level in rice grains for the food security.
Therefore, this paper has been based on understanding of previous studies, the distribution pattern of polluted metals in size fractions was studied in first,anylised the forming of soil aggregates in polluted paddy field and the distribution pattern of polluted metals in size fractions.the effect of heavy metal pollution on the process of biological and physical in soils was discussed;Second, the rice samples was collected from different producing areas in South China,and anylised the contents of Cd, Zn in rice grain.In addition,the relationship between soil type and the characters of soil on rice producing areas was discussed. Finally, this study discussed the technology of reducing Cd accumulation in rice grain through regulation of soil pH, because soil acidity is main facter to affect the heavy metal in rice grain. The main results were as follows:
1.Topsoil samples of polluted and non-polluted rice paddy were respectively collected from the Tai Lake region, China.Particle size fractions of soil micro-aggregates were separated using a low-energy dispersion procedure and the mass composition of these fractions were measured. Concentrations of Pb, Cd, Hg and As of the particle size fractions were determined with atomic adsorption spectroscopy and atomic fluorenscence spectroscopy respectively. The changes in composition of and metal distribution in the particle size fractions with soil pollution were discussed. The content of the sand-sized fractions were reduced while that of the clay-sized increased under heavy metal pollution in the rice paddy. The contents of the analyzed metals followed a similar distribution pattern over the different size fractions although their concentrations differed greatly in a single size fraction. The highest concentration was found in the fraction of<0.002 mm in size followed by the sand-sized fraction of 2-0.2mm. However, all the metals were relatively depleted in the silt fractions of 0.02-0.002 mm and 0.2-0.02 mm. The present study show that aggregation of fine particles into large particles may be depressed under heavy metal pollution which, in turn, leads to relative increase in mass of fine particles and the associated allocation of metals in weakly aggregated silt particles. This could further impact the potential translocation of heavy metals through release in water and air particulate material in air in field.
2.In this study, a total of 70 polished rice were randomly collected at agro-product markets and local farmers from some typical rice areas of South China.Their contents of Cd, Zn and Se were determined by atomic adsorption spectrophotometer (AAS) and astomic fluorescence spectrometry (AFS) respectively, the variation of the contents with rice areas was described in terms of soil conditions.The result showed that over 70% of the total samples have Cd contents exceeding the State Food Security Standards (0.2 mg·kg-1) with Cd/Zn ratios exceeding the suggested critical threshold of 0.015.The extent to which the contents of the analyzed elements varied with rice areas was greater for Cd and Se than for Zn, though the contents followed in the same order:polluted area>acid paddy area and neutral paddy area. This further evidenced a determinacy of soil acidity and Cd availability in rice Cd uptake.Thus, Cd translocation and accumulation in grains could be result from the interactive effect of human activities and the chemical properties of soil. The health risk by Cd exposure to the rice diet from different areas was estimated. The consumption of rice from polluted area and acid paddy area may impose serious health risks for subsistence diet farmers.
3.Based on former result and the effective control measures of soil acidity and taking into account the antagonistic relationship between the.Cd and Zn in soil. A field experiment was conducted to study the effects on grain Cd concentration of different dosages of calcium magnesium phosphate fertilization and foliar ZnSO4·7H2O fertilization. The results showed that most treatments had not significantly increased rice yield but decreased grain Cd concentration with varying extent. The analysis showed that soil pH was increased under all the phosphate fertilizer treatments, in proportional to the application dosage. Accordingly, significant reduction in bioavailable Cd was observed. Statistical analysis indicated a significantly negative correlation of bioavailable Cd with soil pH.Therefore, the reduction in grain Cd concentration under these phosphorus fertilization treatments was attributed to the reduced mobility of soil Cd under increased soil pH. Foliar application of ZnSO4·7H2O solution was not found to increase soil pH, but again decrease soil bioavailable Cd, which was likely to result from the formation of CdS under submerged condition. Therefore, inactivating soil Cd by the pH-increasing phosphorus fertilization and mobility reducing foliar sulphate could alleviate Cd uptake and accumulation in rice grains. However, grain Cd from this heavily polluted paddy was not reduced to meet the National food safety guideline with the studied dosages. It is suggested that alternative crops with low Cd affinity should be cultivated instead of rice for sound agro-production in polluted rice fields.
The study showed that soil pollution in rice field may impact on the basic properties of the soil, also further effect all kinds of processes in soil;at the same time,the effect on food quality in polluted rice fields could be result from the common effects of pollutants quantity and the properties of soil.The difference of soil acidity may be the main facter in rice Cd from different producing rice area. Therefore, adjust and control the soil acidity,research control technique of heavy metal polluted in rice should be taken into account in the future.
因此,本文基于已有认识,首先研究了重金属污染下稻田土壤团聚体组成变化,分析污染下土壤团聚体形成及重金属的土壤颗粒粒径分配变化,探讨重金属污染对土壤生物物理过程的影响；其次,采集南方不同稻区稻米样品,分析Cd、Zn含量,探讨与稻区土壤类型及其土壤性质特征的关系,最后从影响稻区稻米重金属水平的土壤因素-土壤酸度着手,探讨通过施用改良剂调节土壤Cd活性而降低稻米Cd积累的技术。获得结果如下：
1.本文采集已报道严重污染的水稻土和未明显污染的同种水田土壤表土样品,分析不同粒径土壤团聚体颗粒组的质量组成和Pb、Cd、Hg、As等重金属元素的含量,讨论重金属污染下土壤团聚体组成和重金属团聚体分配的变化。在重金属污染下,土壤砂粒级团聚体减少,而较细粒径团聚体相对增多；尽管重金属含量随粒径变化的趋势与先前研究认识一致,即在<0.002mm和2-0.2mm粒径的颗粒组中富集,但污染下重金属元素更多地赋存于粉砂组和黏粒组团聚体。因此,重金属污染可能减弱了较大土壤团聚体形成作用,导致细粒径团聚体的相对增多,从而明显提高重金属元素在易移动的粉砂和黏粒组团聚体的分配,这可能进一步加剧污染农田重金属的水迁移和大气颗粒物迁移的风险。
2.在江西、湖南、安徽和广东等南方典型水稻产区的农产品市场和农户随机采取大米样品共70份,分别测定样品中Cd、Zn和Se的含量,并分析不同产地大米的含量差异及其与产区主要土壤特征的关系。结果表明,70%以上的供试样品Cd含量超出国家食品卫生标准值(0.2mg·kg-1),且Cd/Zn(质量比)超出美国学者建议的0.015临界值。不同产地大米样本间所分析元素的含量及Cd/Zn均呈污染产地>酸性水稻土产地>中性水稻土产地,且以Cd和Se含量的差异幅度较大,Zn较小。说明土壤酸度及Cd有效性是影响供试大米Cd含量的主要因素。因而,土壤-水稻系统中Cd迁移与籽粒积累取决于人为污染和土壤的化学性质的共同作用。分析表明所有供试产地的大米样本对于农民就地消费来说均存在不同程度的潜在Cd暴露风险,以污染土壤产地区和酸性红壤性水稻土产地为严重。
3.根据前述结果,针对土壤酸度对稻米Cd积累的重要影响,并考虑到Cd-Zn拮抗关系和沉淀钝化作用,采用田间定位试验,探讨了不同用量的钙镁磷肥及叶面喷施锌肥(ZnSO4·7H20)等处理对降低污染稻田水稻籽粒Cd含量的影响。试验表明,不同肥料调节剂处理没有显著提高水稻产量,但籽粒Cd含量有不同程度降低。分析表明,磷肥处理提高了土壤的pH值,且随用量而增高,而土壤中有效态Cd含量相应显著降低。推测主要是由于土壤pH升高而降低了土壤Cd活性。不过,叶面喷施锌肥并未明显提高土壤pH值,但显著降低土壤有效态Cd含量,看来淹水下形成难溶性CdS而钝化了土壤Cd。施用磷肥调节剂可以通过调控土壤酸度而达到钝化稻田土壤Cd从而抑制水稻籽粒中Cd积累的效果。但是,在严重污染稻田中,这些用量尚不能有效控制稻米Cd的安全。建议严重重金属污染的土壤改种其它非Cd强积累作物。
本文的研究说明,稻田土壤污染可能影响土壤的物理性质,可能带来对土壤中各种过程的进一步影响；同时,稻田土壤污染对食物安全的影响可能受污染物数量和土壤性质的共同影响,土壤酸度差异可能是产地区域稻米Cd分异的主要因素,因而从土壤酸度调节和控制出发研究稻米重金属污染控制技术是一个今后需要努力的方向。
Soils are the physical support for the terrestrial ecosystem and also the most important component of the earth surface environment. Soil pollution and its health risks via food consumption for human is one of the great challenges for the sustainable agriculture together with the need for increasing soil productivity. Soil pollution, however, is very extensive in South China rice area, especially from the Tai Lake region, Pearl River delta region and red earth region of Jiangxi and Hunan provinces. Many studies on soil pollution of heavy metals such as Pb, Cd, As in rice paddies and the exposure risks by dietary intake have been reported. Among these, a number of studies have been conducted at Institute of Resources, Ecosystem and Environment of Agriculture (IREEA) on soil distribution, accumulation in rice grains and evaluation of food exposure risks from the Tai Lake region, Jiangsu. Whereas, the effect of heavy metals on composition of soil aggregates of different size frcationss, and thus, the distribution pattern of these polluted metals in size fractions has not yet been examed. In addition, the relationship of heavy metal concentration in rice grains with the soil properties where the rice were grown has not been elucidated. And at last, there have not yet been feasible measures for depressing the heavy metal level in rice grains for the food security.
Therefore, this paper has been based on understanding of previous studies, the distribution pattern of polluted metals in size fractions was studied in first,anylised the forming of soil aggregates in polluted paddy field and the distribution pattern of polluted metals in size fractions.the effect of heavy metal pollution on the process of biological and physical in soils was discussed;Second, the rice samples was collected from different producing areas in South China,and anylised the contents of Cd, Zn in rice grain.In addition,the relationship between soil type and the characters of soil on rice producing areas was discussed. Finally, this study discussed the technology of reducing Cd accumulation in rice grain through regulation of soil pH, because soil acidity is main facter to affect the heavy metal in rice grain. The main results were as follows:
1.Topsoil samples of polluted and non-polluted rice paddy were respectively collected from the Tai Lake region, China.Particle size fractions of soil micro-aggregates were separated using a low-energy dispersion procedure and the mass composition of these fractions were measured. Concentrations of Pb, Cd, Hg and As of the particle size fractions were determined with atomic adsorption spectroscopy and atomic fluorenscence spectroscopy respectively. The changes in composition of and metal distribution in the particle size fractions with soil pollution were discussed. The content of the sand-sized fractions were reduced while that of the clay-sized increased under heavy metal pollution in the rice paddy. The contents of the analyzed metals followed a similar distribution pattern over the different size fractions although their concentrations differed greatly in a single size fraction. The highest concentration was found in the fraction of<0.002 mm in size followed by the sand-sized fraction of 2-0.2mm. However, all the metals were relatively depleted in the silt fractions of 0.02-0.002 mm and 0.2-0.02 mm. The present study show that aggregation of fine particles into large particles may be depressed under heavy metal pollution which, in turn, leads to relative increase in mass of fine particles and the associated allocation of metals in weakly aggregated silt particles. This could further impact the potential translocation of heavy metals through release in water and air particulate material in air in field.
2.In this study, a total of 70 polished rice were randomly collected at agro-product markets and local farmers from some typical rice areas of South China.Their contents of Cd, Zn and Se were determined by atomic adsorption spectrophotometer (AAS) and astomic fluorescence spectrometry (AFS) respectively, the variation of the contents with rice areas was described in terms of soil conditions.The result showed that over 70% of the total samples have Cd contents exceeding the State Food Security Standards (0.2 mg·kg-1) with Cd/Zn ratios exceeding the suggested critical threshold of 0.015.The extent to which the contents of the analyzed elements varied with rice areas was greater for Cd and Se than for Zn, though the contents followed in the same order:polluted area>acid paddy area and neutral paddy area. This further evidenced a determinacy of soil acidity and Cd availability in rice Cd uptake.Thus, Cd translocation and accumulation in grains could be result from the interactive effect of human activities and the chemical properties of soil. The health risk by Cd exposure to the rice diet from different areas was estimated. The consumption of rice from polluted area and acid paddy area may impose serious health risks for subsistence diet farmers.
3.Based on former result and the effective control measures of soil acidity and taking into account the antagonistic relationship between the.Cd and Zn in soil. A field experiment was conducted to study the effects on grain Cd concentration of different dosages of calcium magnesium phosphate fertilization and foliar ZnSO4·7H2O fertilization. The results showed that most treatments had not significantly increased rice yield but decreased grain Cd concentration with varying extent. The analysis showed that soil pH was increased under all the phosphate fertilizer treatments, in proportional to the application dosage. Accordingly, significant reduction in bioavailable Cd was observed. Statistical analysis indicated a significantly negative correlation of bioavailable Cd with soil pH.Therefore, the reduction in grain Cd concentration under these phosphorus fertilization treatments was attributed to the reduced mobility of soil Cd under increased soil pH. Foliar application of ZnSO4·7H2O solution was not found to increase soil pH, but again decrease soil bioavailable Cd, which was likely to result from the formation of CdS under submerged condition. Therefore, inactivating soil Cd by the pH-increasing phosphorus fertilization and mobility reducing foliar sulphate could alleviate Cd uptake and accumulation in rice grains. However, grain Cd from this heavily polluted paddy was not reduced to meet the National food safety guideline with the studied dosages. It is suggested that alternative crops with low Cd affinity should be cultivated instead of rice for sound agro-production in polluted rice fields.
The study showed that soil pollution in rice field may impact on the basic properties of the soil, also further effect all kinds of processes in soil;at the same time,the effect on food quality in polluted rice fields could be result from the common effects of pollutants quantity and the properties of soil.The difference of soil acidity may be the main facter in rice Cd from different producing rice area. Therefore, adjust and control the soil acidity,research control technique of heavy metal polluted in rice should be taken into account in the future.
引文
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