长三角地区土壤—小麦系统微量元素迁移的地球化学特征
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摘要
随着社会的发展,土壤——农作物系统重金属等有害元素污染已成为热点环境问题。自上个世纪中期以来,研究人员开展了许多围绕农业土壤系统中重金属污染来源的调查以及元素生物有效性等问题开展了许多调查和实验研究,尽管如此,人们对区域实际条件下重金属尤其是氟、硒、钼、硼等微量元素在土壤——农作物体系中迁移和富集的机理以及影响因素的研究尚不足；对微量元素同位素在地表系统中迁移活性的研究很少；在土壤环境中微量元素的微观原位分析研究领域尚处于探索发展阶段。
长三角地区作为我国重要的经济发展区域,其生态环境受到了工业农业快速发展带来的破坏。虽然近几年来,我国相关单位和科研工作者针对该地区的生态环境污染做了许多研究,但在全区域范围内的土壤和小麦中微量元素地球化学行为特征的调查研究较为少见。长三角地区表层土壤和小麦具有怎样的元素含量和空间分布以及富集特征,在实际农业系统中微量元素从土壤到小麦中的迁移受哪些因素的影响,有害元素在污染的土壤和小麦籽实中微米层次的赋存位置以及与相关元素的关系等一系列问题尚有待于研究。
本研究选择长三角地区为研究区域,以土壤和小麦为主要研究对象(包括相关圈层物质),通过野外调查和采样、实验数据分析和综合研究,系统研究了微量元素在土壤——小麦系统中迁移的地球化学行为特征,获得了以下主要认识：
(1)长三角地区表层土壤相对于中国土壤平均水平有较高的Cu、Cd、Zn、Hg、F含量、相近的Pb、Ni、Cr、Se和B含量以及较低的As和Mo含量；相对于世界土壤平均水平具有较高的Cu、Hg、As、B和F含量,Zn和Cr的平均含量与世界水平基本一致,Cd、Pb、Ni、Se和Mo含量低于世界平均水平。研究区表层土壤在过去几十年中发生了Cd、Cu、Zn、Cr、Ni和F富集,各重金属富集程度的排序为Cd>Cu>Zn>Cr>Ni>As>Hg>Pb。根据我国土壤质量标准,研究区耕层土壤各重金属的污染率依次是Cd>Hg>Cu=Zn>Cr>Ni>Pb>As。总体来说,苏州和杭州——嘉兴地区的表层土壤呈现除As外的7种重金属、F和B明显的富集。
(2)土壤Cd、Cu、Zn、Hg、Ni和Cr富集(污染)主要是受冶炼、电镀、化工等工业排放影响的缘故,F富集可能主要是源自石料、水泥等与成土母质有关的人为活动带来的输入,Mo、Se和As富集主要与富硒岩石、煤等的使用开发带来的废弃物扩散有关,而Pb的富集源则与其它元素不同,可能是主要直接受大气沉降影响造成的。
(3)长三角地区小麦籽实发生了F、Zn、Cd、Cu、Ni、Pb以及Hg污染,污染主要分布在苏南和浙北地区。根据籽实样品污染率,各污染物次序为F>Ni>Zn>Cd=Cu>Pb>Hg>As>Se>Cr。微量元素不同的小麦组织的含量具有很大的差异：As、Pb、Cd、Ni、Cr、F和Se在小麦植株不同部位中的含量遵从根>秸秆>籽实的顺序,Cu、Hg和B遵从秸秆>根>籽实的次序,Zn和Mo遵从籽实>秸秆>根的次序。
(4)根据元素从土壤到小麦根部、再到秸秆、籽实整个过程的迁移系数以及迁移模式的变化特征,可以将全部元素分为三类。第一类主要包括Hg、Pb、Cu、 As、Cr、Mo、F和B,迁移系数先增加后减小,整个迁移过程曲线呈“峰”型,表明小麦根和籽实对于吸收这些元素具有较明显的排斥,主要反映了大气对小麦秸秆和叶片中这些元素含量的贡献。相关分析表明籽实中氟主要来自秸秆,但小麦秸秆和籽实中F的主要来源不是土壤,而可能是大气。第二类为迁移能力步步增长型,即迁移系数从土壤→根、根→秸秆、再到秸秆→籽实逐步增大,主要包括Zn、Ni、Cd、Se和P,体现了这些元素的强迁移能力。S和Fe被归为第三类,属于特殊型。
(5)回归和通径分析表明,长三角地区土壤重金属本身及其有效态、pH、土壤铵态氮、缓效钾、碳酸盐、活性二价阳离子是影响小麦从土壤中吸收重金属、Mo和B最主要的影响因素。耕层土壤pH、Ca、Mg、碳酸盐和缓效钾能抑制重金属从土壤向小麦中迁移；而土壤重金属本身以及其它重金属、Ex-Ca、Ex-Mg、有效Fe、铵态氮对重金属从土壤向小麦籽实中迁移表现出促进作用。土壤Se、Mo、有效Mo、pH、S、酸可溶Al、碳酸盐和P含量的增加能促进小麦吸收土壤中的Se和Mo,小麦从土壤中吸收B主要受控于土壤总硼和有效硼。
(6)碳酸盐对小麦吸收土壤中重金属的遏制作用是不同的,依次为：Ni>Zn>Cd>Cu>Pb>Fe≈Cr≈Hg.在贫(无)碳酸盐土壤上种植的小麦具有明显较高的Ni、Cd等重金属含量。研究区大部分土壤样品(镇江沿江地区的样品除外)发生了严重的碳酸盐淋失,含有碳酸盐样品的碳氧同位素分析表明土壤中的碳酸盐主要是原生海相碳酸盐。
(7)铅在不同环境介质具有不同的或互相叠加的同位素组成特征,但是无论是在人为源还是自然源中,Pb同位素分配大致遵循下述方程：208pb/206pb=-1.157×206Pb/207Pb+3.460(r2=0.941).长三角地区人为端元Pb相对富集重铅,与当地出产的铅矿石Pb同位素分布范围基本一致。深层土壤相对于地层沉积岩具有较低的208Pb/206Pb比值和略高的206pb/207pb,说明在成土过程中,轻铅(206pb)更倾向于从岩石中风化释放进入土壤圈。土壤可交换态Pb和碳酸盐态Pb相对于总铅具有明显低的206pb/207pb比值,人为铅对表层土壤中可交换Pb和碳酸盐态Pb的存在有重要影响。轻铅在土壤中的活性比重铅强,优先进入可交换态,向深部迁移；在深部的淀积层重铅则较轻铅优先与碳酸盐结合沉淀。水稻倾向于吸收和积累较轻的206pb同位素；但是由于大气沉降Pb污染对水稻吸收Pb的影响,造成了长三角地区水稻籽实比根富集重铅(208pb)的现象。通过Pb同位素识别污染源模型估算,长三角地区水稻籽实中大约有16.7-52.6%(平均33.5%)的Pb为大气成因。
(8)土壤样品中重金属元素的空间微区分布与Fe基本一致,与Mg和Mn比较一致。二价阳离子重金属可能主要以置换形式与土壤中Fe、Mg等阳离子发生替代,以黏粒——细粒被土壤铁氧化物和黏土矿物所吸附固定于土壤固相之中。小麦籽实的NanoSIMS扫描图像表明,Si主要分布在淀粉颗粒和糊粉细胞的细胞壁层中；氟在表皮、糊粉细胞和胚乳层的淀粉颗粒以及蛋白质基质中皆有一定分布,氟在小麦籽实的各个组织细胞中是普遍存在的。小麦籽实中Fe和Zn的分布极为类似,与P和O-H关系密切,说明K、Mg、Ca、Fe和Zn在小麦籽实中主要以植酸和多糖的物种存在。重金属在土壤——小麦系统中的地球化学行为与其本身及Fe等相关元素的生物地球化学活性有密切关系。
Heavy metals contamination of soil and agro-products is an important issue with the increasing anthropogenic activities. There have been increasing studies on the heavy metals contamination of soil and plant. However, many questions about the geochemical behavior of trace elements in soil-plant are still unclear due to the complexity of the soil-plant system. Although many previous researches have studied the source of the contamination and the bio-availability of the heavy metals in soil with special experiments, the knowledge on the transfer and accumulation of fluorine, selenium, molybdenum, boron and other trace elements in the soil-plant and the influence factor is scant, so is the knowledge on the mobility of the trace isotopes transfer in the terrestrial system and in situ examination of trace elements in soil and plant at the micrometer level.
The ecological environment of the Yangtze River delta area has been deteriorating with the accelerated economic develop in the past few decades. Although some researchers have investigated the environment pollution of heavy metals in this region, the study on the geochemical characteristics of trace elements in the soil-wheat system on a whole regional scale is lacking. What are characteristics of the concentrations (or accumulations) of trace elements and their spatial distributions? What do soil parameters effect the process of trace elements transfer from soil to wheat and which are the main influence factors? How do trace elements in the contaminated soil and wheat grain distribute at the micrometer scale? These questions need to be answered through the study of a representative area in the Yangtze River delta. The candidate selected the Yangtze River delta region as the study area and used the soil and wheat as the major study objects, and combined the field investigation, laboratory measurements and datum analyses, to characterize the geochemical behavior of trace elements in the soil-wheat system. The main results and conclusions are summarized below:
(1) The topsoils of the Yangtze River delta region show relatively higher concentrations of Cu, Cd, Zn, Hg and F, similar concentrations of Pb, Ni, Cr, Se and B, and lower concentrations of As and Mo than the average level of Chinese topsoil. Comparing to average elemental concentration of the world soil, the soil in the study area has higher concentrations of Cu, Hg, As, B and F, similar concentrations of Zn and Cr, and lower concentrations of Cd, Pb, Ni, Se and Mo. The topsoil has accumulated a relatively higher amount of Cd, Cu, Zn, Cr, Ni and F during the past decades. The rate of heavy metals pollution is in the order of Cd> Hg> Cu=Zn> Cr> Ni> Pb> As. The spatial distributions of trace elements are not the same. In general, the topsoil from Suzhou and Hangzhou-Jiaxing area show apparent accumulation and pollution of heavy metals (except for As), F and B.
(2) The accumulation (contamination) of Cd, Cu, Zn, Hg, Ni and Cr of the topsoil mainly came from metallurgy, electroplate and other industrial emission. The accumulation of F was a closely related to the stone mining and manufacturing and other relative anthropogenic activities. The accumulation of Mo, Se and As might be due to the exploration of local pedogenic parent rock and coal. And the accumulation of Pb may be a result of the increasing atmosphere deposition.
(3) The wheat grain from the Yangtze River delta region shows general to severe F, Zn, Cd, Cu, Ni, Pb and Hg pollution, and the contamination is generally distributed in the south of Jiangsu and the north of Zhejiang. The contamination rates were in the order of F> Ni> Zn> Cd=Cu> Pb> Hg> As> Se> Cr. Different wheat tissues show different in elemental concentrations:As, Pb, Cd, Ni, Cr, F, Se and Fe concentrations follow root> straw> grain, Cu, Hg and B follow straw> root> grain, Zn and Mo follow grain> straw> root.
(4) According to the difference of the transfer coefficient and the transfer model, all the elements can be divided into three groups. The first group includes Hg, Pb, Cu, As, Cr, Mo, F and B. Their transfer coefficient increases from the soil to the straw, then decreases from the straw to the grain. The whole transfer model shows "convex" pattern, indicating that wheat has a low tendency on absorbing these elements. This pattern mainly reflects the atmospheric component to the accumulation of Hg, Pb, Cu, As, Cr, Mo, F and B in wheat straw and grain. The second group includes Zn, Ni, Cd, Se and P, the element transfer coefficient increases step by step, i.e., increases from soil to wheat grain via root and straw. This pattern mainly reflects the strong transfer abilities of these elements.
(5) Soil pH, Ca, Mg, TOC, carbonate and slowly available potassium hinder the heavy metals transfer from soil to wheat, whereas Ex-Ca, Ex-Mg, bio-available Fe, ammonium nitrogen and heavy metal themselves present the promote the transfer. Increasing the concentrations of Soil Se, Mo, bio-available Mo, S, oxalic acid extractable Al, carbonate, TOC, P and pH can enhance the accumulation of Se and Mo in the wheat. Boron absorption and accumulation in the wheat is mainly affected by soil B and bio-available B. Regression and partial correlation analysis show that besides the concentrations of heavy metal and its bio-availability and soil pH, soil ammonium nitrogen, slowly available potassium, carbonate, active bivalent cations and available phosphorus are the most important influence factors on the transfer of heavy metals, Mo and B from soil to wheat.
(6) The effect of carbonate on the transfer of heavy metals from soil to wheat is different:Ni> Zn> Cd> Cu> Pb> Fe≈Cr≈Hg. Higher soil carbonate content will increase the absorption of Se and Mo in the wheat. Most of the topsoil samples from the Yangtze River delta area had lost carbonate, the carbon and oxygen isotopic analyses on the carbonate contained soil sample shows that the carbonate in the topsoil is mainly marine primary carbonate origin.
(7) Pb isotopes have different mobility in different environmental matrixes. Pb isotopes in the geochemical cycle generally follow the equation of208Pb/206Pb=-1.157×206Pb/207Pb+3.46(r2=0.941). The anthropogenic Pb has the lower206Pb/207Pb (1.11-1.17)and relatively higher208Pb/206Pb (2.07-2.18), i.e., enriched in relatively heavy Pb isotopes, and the range of Pb isotopic ratios of anthropogenic Pb is similar to that of the local Pb ore. During the pedogenic process, the lighter Pb (206Pb) is more likely to transport into soil from the parent rock. Soil exchangeable Pb and carbonates phase Pb show the lower206Pb/207Pb relative to the total Pb, indicating that the anthropogenic Pb has an important effect on the existence of exchangeable Pb and carbonate phase Pb in the topsoil. In the pedosphere, the lighter Pb (206Pb) usually shows stronger mobility relative to the heavier Pb (208Pb), and is more likely to transfer into the soil exchangeable Pb fraction and move deeper, whereas heavier Pb has a priority to precipitate with carbonate in the deeper sediment horizon compared to the lighter Pb. The lighter Pb shows stronger transfer ability from soil to cereal grain via root compared to the heavier Pb. However, the cereal grains have lower206Pb/207Pb and higher208Pb/206Pb airborne Pb and anthropogenic Pb, implying that a considerable amount of Pb in cereal grains comes from the atmosphere. The model shows that16.7-52.6%(average:33.5%) of Pb in rice grain is the airborne Pb.
(8) The spatial distributions of heavy metals at micrometer level are the most similar to that of Fe, next similar to that of Mg and Mn. This indicates that heavy metals have a similar distribution at the microcosmic level in the soil, mainly co-existing with Fe. Active bivalent heavy metal cations may mainly exist as isomorphs with Fe, Mg and other bivalent cations. They form into the compounds as the fine-grained clay-granule and been absorbed in the iron oxides, clays, and other soil solid. NanoSIMS images show that Si mainly distributes in the starch granules and cell wall of the aleurone. F generally distributes in the epidermis, aleurone and both starch granules and protein matrix of endosperm. Zn, Fe, Mg, Ca and K in the wheat grain mainly exist in the phytate granules of aleurone. The SIMS image of Zn is very similar to that of Fe, and Zn has a close relationship with P and O-H, implying that Zn, Fe, Mg, Ca and K in the wheat grain mainly coexist with phytic acid and polysaccharides.
长三角地区作为我国重要的经济发展区域,其生态环境受到了工业农业快速发展带来的破坏。虽然近几年来,我国相关单位和科研工作者针对该地区的生态环境污染做了许多研究,但在全区域范围内的土壤和小麦中微量元素地球化学行为特征的调查研究较为少见。长三角地区表层土壤和小麦具有怎样的元素含量和空间分布以及富集特征,在实际农业系统中微量元素从土壤到小麦中的迁移受哪些因素的影响,有害元素在污染的土壤和小麦籽实中微米层次的赋存位置以及与相关元素的关系等一系列问题尚有待于研究。
本研究选择长三角地区为研究区域,以土壤和小麦为主要研究对象(包括相关圈层物质),通过野外调查和采样、实验数据分析和综合研究,系统研究了微量元素在土壤——小麦系统中迁移的地球化学行为特征,获得了以下主要认识：
(1)长三角地区表层土壤相对于中国土壤平均水平有较高的Cu、Cd、Zn、Hg、F含量、相近的Pb、Ni、Cr、Se和B含量以及较低的As和Mo含量；相对于世界土壤平均水平具有较高的Cu、Hg、As、B和F含量,Zn和Cr的平均含量与世界水平基本一致,Cd、Pb、Ni、Se和Mo含量低于世界平均水平。研究区表层土壤在过去几十年中发生了Cd、Cu、Zn、Cr、Ni和F富集,各重金属富集程度的排序为Cd>Cu>Zn>Cr>Ni>As>Hg>Pb。根据我国土壤质量标准,研究区耕层土壤各重金属的污染率依次是Cd>Hg>Cu=Zn>Cr>Ni>Pb>As。总体来说,苏州和杭州——嘉兴地区的表层土壤呈现除As外的7种重金属、F和B明显的富集。
(2)土壤Cd、Cu、Zn、Hg、Ni和Cr富集(污染)主要是受冶炼、电镀、化工等工业排放影响的缘故,F富集可能主要是源自石料、水泥等与成土母质有关的人为活动带来的输入,Mo、Se和As富集主要与富硒岩石、煤等的使用开发带来的废弃物扩散有关,而Pb的富集源则与其它元素不同,可能是主要直接受大气沉降影响造成的。
(3)长三角地区小麦籽实发生了F、Zn、Cd、Cu、Ni、Pb以及Hg污染,污染主要分布在苏南和浙北地区。根据籽实样品污染率,各污染物次序为F>Ni>Zn>Cd=Cu>Pb>Hg>As>Se>Cr。微量元素不同的小麦组织的含量具有很大的差异：As、Pb、Cd、Ni、Cr、F和Se在小麦植株不同部位中的含量遵从根>秸秆>籽实的顺序,Cu、Hg和B遵从秸秆>根>籽实的次序,Zn和Mo遵从籽实>秸秆>根的次序。
(4)根据元素从土壤到小麦根部、再到秸秆、籽实整个过程的迁移系数以及迁移模式的变化特征,可以将全部元素分为三类。第一类主要包括Hg、Pb、Cu、 As、Cr、Mo、F和B,迁移系数先增加后减小,整个迁移过程曲线呈“峰”型,表明小麦根和籽实对于吸收这些元素具有较明显的排斥,主要反映了大气对小麦秸秆和叶片中这些元素含量的贡献。相关分析表明籽实中氟主要来自秸秆,但小麦秸秆和籽实中F的主要来源不是土壤,而可能是大气。第二类为迁移能力步步增长型,即迁移系数从土壤→根、根→秸秆、再到秸秆→籽实逐步增大,主要包括Zn、Ni、Cd、Se和P,体现了这些元素的强迁移能力。S和Fe被归为第三类,属于特殊型。
(5)回归和通径分析表明,长三角地区土壤重金属本身及其有效态、pH、土壤铵态氮、缓效钾、碳酸盐、活性二价阳离子是影响小麦从土壤中吸收重金属、Mo和B最主要的影响因素。耕层土壤pH、Ca、Mg、碳酸盐和缓效钾能抑制重金属从土壤向小麦中迁移；而土壤重金属本身以及其它重金属、Ex-Ca、Ex-Mg、有效Fe、铵态氮对重金属从土壤向小麦籽实中迁移表现出促进作用。土壤Se、Mo、有效Mo、pH、S、酸可溶Al、碳酸盐和P含量的增加能促进小麦吸收土壤中的Se和Mo,小麦从土壤中吸收B主要受控于土壤总硼和有效硼。
(6)碳酸盐对小麦吸收土壤中重金属的遏制作用是不同的,依次为：Ni>Zn>Cd>Cu>Pb>Fe≈Cr≈Hg.在贫(无)碳酸盐土壤上种植的小麦具有明显较高的Ni、Cd等重金属含量。研究区大部分土壤样品(镇江沿江地区的样品除外)发生了严重的碳酸盐淋失,含有碳酸盐样品的碳氧同位素分析表明土壤中的碳酸盐主要是原生海相碳酸盐。
(7)铅在不同环境介质具有不同的或互相叠加的同位素组成特征,但是无论是在人为源还是自然源中,Pb同位素分配大致遵循下述方程：208pb/206pb=-1.157×206Pb/207Pb+3.460(r2=0.941).长三角地区人为端元Pb相对富集重铅,与当地出产的铅矿石Pb同位素分布范围基本一致。深层土壤相对于地层沉积岩具有较低的208Pb/206Pb比值和略高的206pb/207pb,说明在成土过程中,轻铅(206pb)更倾向于从岩石中风化释放进入土壤圈。土壤可交换态Pb和碳酸盐态Pb相对于总铅具有明显低的206pb/207pb比值,人为铅对表层土壤中可交换Pb和碳酸盐态Pb的存在有重要影响。轻铅在土壤中的活性比重铅强,优先进入可交换态,向深部迁移；在深部的淀积层重铅则较轻铅优先与碳酸盐结合沉淀。水稻倾向于吸收和积累较轻的206pb同位素；但是由于大气沉降Pb污染对水稻吸收Pb的影响,造成了长三角地区水稻籽实比根富集重铅(208pb)的现象。通过Pb同位素识别污染源模型估算,长三角地区水稻籽实中大约有16.7-52.6%(平均33.5%)的Pb为大气成因。
(8)土壤样品中重金属元素的空间微区分布与Fe基本一致,与Mg和Mn比较一致。二价阳离子重金属可能主要以置换形式与土壤中Fe、Mg等阳离子发生替代,以黏粒——细粒被土壤铁氧化物和黏土矿物所吸附固定于土壤固相之中。小麦籽实的NanoSIMS扫描图像表明,Si主要分布在淀粉颗粒和糊粉细胞的细胞壁层中；氟在表皮、糊粉细胞和胚乳层的淀粉颗粒以及蛋白质基质中皆有一定分布,氟在小麦籽实的各个组织细胞中是普遍存在的。小麦籽实中Fe和Zn的分布极为类似,与P和O-H关系密切,说明K、Mg、Ca、Fe和Zn在小麦籽实中主要以植酸和多糖的物种存在。重金属在土壤——小麦系统中的地球化学行为与其本身及Fe等相关元素的生物地球化学活性有密切关系。
Heavy metals contamination of soil and agro-products is an important issue with the increasing anthropogenic activities. There have been increasing studies on the heavy metals contamination of soil and plant. However, many questions about the geochemical behavior of trace elements in soil-plant are still unclear due to the complexity of the soil-plant system. Although many previous researches have studied the source of the contamination and the bio-availability of the heavy metals in soil with special experiments, the knowledge on the transfer and accumulation of fluorine, selenium, molybdenum, boron and other trace elements in the soil-plant and the influence factor is scant, so is the knowledge on the mobility of the trace isotopes transfer in the terrestrial system and in situ examination of trace elements in soil and plant at the micrometer level.
The ecological environment of the Yangtze River delta area has been deteriorating with the accelerated economic develop in the past few decades. Although some researchers have investigated the environment pollution of heavy metals in this region, the study on the geochemical characteristics of trace elements in the soil-wheat system on a whole regional scale is lacking. What are characteristics of the concentrations (or accumulations) of trace elements and their spatial distributions? What do soil parameters effect the process of trace elements transfer from soil to wheat and which are the main influence factors? How do trace elements in the contaminated soil and wheat grain distribute at the micrometer scale? These questions need to be answered through the study of a representative area in the Yangtze River delta. The candidate selected the Yangtze River delta region as the study area and used the soil and wheat as the major study objects, and combined the field investigation, laboratory measurements and datum analyses, to characterize the geochemical behavior of trace elements in the soil-wheat system. The main results and conclusions are summarized below:
(1) The topsoils of the Yangtze River delta region show relatively higher concentrations of Cu, Cd, Zn, Hg and F, similar concentrations of Pb, Ni, Cr, Se and B, and lower concentrations of As and Mo than the average level of Chinese topsoil. Comparing to average elemental concentration of the world soil, the soil in the study area has higher concentrations of Cu, Hg, As, B and F, similar concentrations of Zn and Cr, and lower concentrations of Cd, Pb, Ni, Se and Mo. The topsoil has accumulated a relatively higher amount of Cd, Cu, Zn, Cr, Ni and F during the past decades. The rate of heavy metals pollution is in the order of Cd> Hg> Cu=Zn> Cr> Ni> Pb> As. The spatial distributions of trace elements are not the same. In general, the topsoil from Suzhou and Hangzhou-Jiaxing area show apparent accumulation and pollution of heavy metals (except for As), F and B.
(2) The accumulation (contamination) of Cd, Cu, Zn, Hg, Ni and Cr of the topsoil mainly came from metallurgy, electroplate and other industrial emission. The accumulation of F was a closely related to the stone mining and manufacturing and other relative anthropogenic activities. The accumulation of Mo, Se and As might be due to the exploration of local pedogenic parent rock and coal. And the accumulation of Pb may be a result of the increasing atmosphere deposition.
(3) The wheat grain from the Yangtze River delta region shows general to severe F, Zn, Cd, Cu, Ni, Pb and Hg pollution, and the contamination is generally distributed in the south of Jiangsu and the north of Zhejiang. The contamination rates were in the order of F> Ni> Zn> Cd=Cu> Pb> Hg> As> Se> Cr. Different wheat tissues show different in elemental concentrations:As, Pb, Cd, Ni, Cr, F, Se and Fe concentrations follow root> straw> grain, Cu, Hg and B follow straw> root> grain, Zn and Mo follow grain> straw> root.
(4) According to the difference of the transfer coefficient and the transfer model, all the elements can be divided into three groups. The first group includes Hg, Pb, Cu, As, Cr, Mo, F and B. Their transfer coefficient increases from the soil to the straw, then decreases from the straw to the grain. The whole transfer model shows "convex" pattern, indicating that wheat has a low tendency on absorbing these elements. This pattern mainly reflects the atmospheric component to the accumulation of Hg, Pb, Cu, As, Cr, Mo, F and B in wheat straw and grain. The second group includes Zn, Ni, Cd, Se and P, the element transfer coefficient increases step by step, i.e., increases from soil to wheat grain via root and straw. This pattern mainly reflects the strong transfer abilities of these elements.
(5) Soil pH, Ca, Mg, TOC, carbonate and slowly available potassium hinder the heavy metals transfer from soil to wheat, whereas Ex-Ca, Ex-Mg, bio-available Fe, ammonium nitrogen and heavy metal themselves present the promote the transfer. Increasing the concentrations of Soil Se, Mo, bio-available Mo, S, oxalic acid extractable Al, carbonate, TOC, P and pH can enhance the accumulation of Se and Mo in the wheat. Boron absorption and accumulation in the wheat is mainly affected by soil B and bio-available B. Regression and partial correlation analysis show that besides the concentrations of heavy metal and its bio-availability and soil pH, soil ammonium nitrogen, slowly available potassium, carbonate, active bivalent cations and available phosphorus are the most important influence factors on the transfer of heavy metals, Mo and B from soil to wheat.
(6) The effect of carbonate on the transfer of heavy metals from soil to wheat is different:Ni> Zn> Cd> Cu> Pb> Fe≈Cr≈Hg. Higher soil carbonate content will increase the absorption of Se and Mo in the wheat. Most of the topsoil samples from the Yangtze River delta area had lost carbonate, the carbon and oxygen isotopic analyses on the carbonate contained soil sample shows that the carbonate in the topsoil is mainly marine primary carbonate origin.
(7) Pb isotopes have different mobility in different environmental matrixes. Pb isotopes in the geochemical cycle generally follow the equation of208Pb/206Pb=-1.157×206Pb/207Pb+3.46(r2=0.941). The anthropogenic Pb has the lower206Pb/207Pb (1.11-1.17)and relatively higher208Pb/206Pb (2.07-2.18), i.e., enriched in relatively heavy Pb isotopes, and the range of Pb isotopic ratios of anthropogenic Pb is similar to that of the local Pb ore. During the pedogenic process, the lighter Pb (206Pb) is more likely to transport into soil from the parent rock. Soil exchangeable Pb and carbonates phase Pb show the lower206Pb/207Pb relative to the total Pb, indicating that the anthropogenic Pb has an important effect on the existence of exchangeable Pb and carbonate phase Pb in the topsoil. In the pedosphere, the lighter Pb (206Pb) usually shows stronger mobility relative to the heavier Pb (208Pb), and is more likely to transfer into the soil exchangeable Pb fraction and move deeper, whereas heavier Pb has a priority to precipitate with carbonate in the deeper sediment horizon compared to the lighter Pb. The lighter Pb shows stronger transfer ability from soil to cereal grain via root compared to the heavier Pb. However, the cereal grains have lower206Pb/207Pb and higher208Pb/206Pb airborne Pb and anthropogenic Pb, implying that a considerable amount of Pb in cereal grains comes from the atmosphere. The model shows that16.7-52.6%(average:33.5%) of Pb in rice grain is the airborne Pb.
(8) The spatial distributions of heavy metals at micrometer level are the most similar to that of Fe, next similar to that of Mg and Mn. This indicates that heavy metals have a similar distribution at the microcosmic level in the soil, mainly co-existing with Fe. Active bivalent heavy metal cations may mainly exist as isomorphs with Fe, Mg and other bivalent cations. They form into the compounds as the fine-grained clay-granule and been absorbed in the iron oxides, clays, and other soil solid. NanoSIMS images show that Si mainly distributes in the starch granules and cell wall of the aleurone. F generally distributes in the epidermis, aleurone and both starch granules and protein matrix of endosperm. Zn, Fe, Mg, Ca and K in the wheat grain mainly exist in the phytate granules of aleurone. The SIMS image of Zn is very similar to that of Fe, and Zn has a close relationship with P and O-H, implying that Zn, Fe, Mg, Ca and K in the wheat grain mainly coexist with phytic acid and polysaccharides.
引文
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