土壤和道路沉积物中重金属的释放行为与固定研究
摘要
随着社会经济的快速发展,我国土壤、道路沉积物中的重金属污染日益严重,相关问题已引起人们的密切关注。污染土壤的重金属除了可在土壤-植物系统中迁移转化,影响植物的生长及农产品安全,也可通过地表径流、淋溶等作用逐渐向水体(包括地表和地下水体)迁移,从而对水体的水质、生态环境产生影响。土壤物质可经各种方式搬运成为道路沉积物,后者中的重金属在一定条件下可重新随地表径流迁移。为了解土壤和道路沉积物中重金属向水体的释放潜力、迁移规律、影响因素以及固定污染土壤中重金属的方法,本文通过采样分析、室内模拟试验和田间采样观察等方式,研究了土壤和道路沉积物中重金属积累对水体的潜在影响,分析了土壤重金属释放迁移规律及其与土壤性质的关系,探讨了可表征土壤重金属释放潜力的测试方法,在此基础上探索了降低土壤重金属释放潜力的改良方法。研究获得的初步结果对开展土壤和道路沉积物中重金属对水体的污染风险评估,为今后建立适合水质安全的土壤重金属污染的表征方法,以及控制土壤重金属污染对水体的危害具有一定意义。主要研究结果如下：
1采集了16个稻田土壤,进行为期12个月的Cd、Pb的添加培养试验,通过测定所培养土壤中水溶态和交换态Cd、Pb评估了土壤Cd、Pb的释放行为。结果表明,随着Cd和Pb污染水平的提高,土壤中水溶态和交换态Cd和Pb占全量比例呈增加趋势。未加外源Cd时,水溶态Cd占全Cd的比例平均为0.16%,交换态Cd占全Cd的比例平均为7.24%。外源Cd加入量为0.2、0.5、1.0、2.0和5.0mg·kg-1的处理对应的土壤水溶态Cd占全Cd比例平均分别为0.14%、0.25%、0.34%、0.50%和0.81%；土壤交换态Cd占全Cd比例平均分别为10.73%、11.61%、14.11%、12.55%和10.67%。未加外源Pb时,水溶态Pb占全Pb的比例平均为0.006%,交换态Pb占全Pb的比例平均为0.70%,外源Pb加入量为20.0、50.0、100.0、200.0和500.0mg·kg-1的处理对应土壤水溶态Pb占全Pb比例平均分别为0.008%、0.014%、0.027%、0.036%和0.047%,土壤交换态Pb占全Pb比例平均分别为1.03%、1.71%、2.67%、3.74%和3.84%。不同土壤中水溶态和交换态Cd和Pb含量随土壤Cd和Pb积累的增加幅度有很大的差异。相关分析表明,土壤中水溶性Cd和Pb含量主要与土壤土壤pH、盐基饱和度有关；而交换态Cd和Pb含量主要与pH、盐基饱和度、CEC及土壤质地等有关。pH、CEC较高、质地较粘、盐基饱和度较高的土壤中水溶态、交换态Cd和Pb含量增加幅度较小,可较大程度地降低进入土壤Cd和Pb的释放潜力及对水体的威胁。土壤降低Pb易释放形态的作用高于Cd。
2在杭州选择了5种不同土地利用区(工业区、商业区、居民区、公园、农村),采集了25个道路沉积物样品,测定了样品中重金属的全量,并采用BCR提取法对重金属进行形态分级。结果表明,Cu、Cd、Pb和Zn等元素的富集因子(EF)较高,受人为来源的污染影响较大。由于受交通等污染源的影响,工业区和商业区道路沉积物中重金属含量较高,居民区、公园、农村的重金属含量较低。由BCR提取法的结果可知,道路沉积物中Zn、Cd、Cu和Pb等重金属有较大的释放潜力,对水体环境具有较大潜在威胁。
另在浙北平原选择了63个区块的代表性水田、蔬菜地、果园、苗木地和城市用地,通过收集地表径流,测定地表径流中水溶性Cu、Cd、Pb、Zn、Co、Cr、Fe、Ni、Mn的浓度,同时采集对应区块地表土壤,测定重金属含量,并用0.01mol·L-1CaCl_2溶液测定了土壤水溶态重金属含量。研究结果表明,地表径流中重金属元素平均浓度由低至高依次为Cd、Co、Cr、Ni、Pb、Cu、Zn、Mn和Fe,分别为0.19、0.46、1.04、1.73、4.98、88.47、184.52、609.52和1135.21μg·L-1, Cu、Zn和Pb对水体环境威胁相对较大。径流中Fe和Mn的浓度以水田为最高,Cu的浓度以果园为最高,Cd、Co、Cr、Ni、Pb和Zn的浓度以城区为最高,表明土壤中重金属释放强度与土地利用类型有关。地表径流中水溶性重金属浓度与土壤pH呈极显著或显著负相关,与相应土壤重金属全量和CaCl_2提取态呈极显著或显著的正相关,相比全量土壤CaCl_2提取态重金属含量更能反映土壤重金属随地表径流的流失潜力。随着土壤重金属的积累,特别是活性较高的重金属含量提高,有更多的重金属可通过地表径流流失,对水体水质会产生更大危害。
3用PVC管采集了13个具有不同污染程度的原状土柱,用去离子水进行淋溶,以10mm·h-1的速度模拟1次降雨淋溶过程,淋溶量为50mm。结果表明,淋出液中水溶态Cu、Cd、Pb和Zn占其全量的比例平均分别为25.25%、47.52%、15.45%和35.65%,大部分淋出液中水溶态重金属的浓度低于颗粒态。淋出液中水溶态、颗粒态、全量Cu、Cd、Pb、Zn浓度与土壤容重均呈负相关,水溶态、全量Cu、Cd、Pb、Zn与土壤pH一般呈极显著负相关,颗粒态Cu、Cd、Pb、Zn与pH的相关性不显著,水溶态、颗粒态、全量Cu、Cd、 Pb、Zn与土壤碳酸钙含量及土壤粘粒、有机碳含量和CEC呈负相关。土壤重金属主要以颗粒态垂直淋迁,土壤容重、pH、CEC、粘粒、有机碳是影响土壤重金属淋溶形态的重要性质。
采用受到Cu、Cd、Pb、Zn、Cr较明显污染的土壤进行了添加有机物和酸化2类处理对土壤重金属形态和释放潜力影响的研究,有机物的加入量设0、50、100和200g·kg-14个等级,酸化包括对照和使土壤pH分别降至6、5、4等4个处理,培养1午后进行淋溶试验(淋溶试验共进行17d,每4d淋溶1次,共5次,每次用100m1去离子水淋溶),并用Amacher连续提取法分析土壤重金属的形态变化。结果发现,不加酸而加入0、50、100、200g·kg1的有机物料培养后,土壤pH分别从7.1降为7.0、6.8、6.8和6.7,表明有机质的积累可使土壤pH轻微下降。pH下降可使重金属交换态比例显著增加,其中对Cd、Zn的影响最为明显。pH降至6时,淋出液中Pb、Cu比对照增加了46%-128%, Cd、Zn比对照增加了219%-630%,Cr增加了10%-119%。pH降至5时,淋出液中Cu、Cd、Pb、 Zn、Cr浓度分别比对照增加了165%-555%、156%-940%、196%-475%、214%-746%、70%-444%,pH降至4时各处理淋出液中重金属浓度都达到了很高水平。表明土壤酸化可增加重金属的活性和释放。有机质积累对重金属释放潜力的影响与pH和有机质积累程度有关,当pH较高时,低量有机质的积累可促进重金属的释放,高量有机质的积累可减少重金属的释放；而当pH较低时,有机质的积累可降低土壤重金属的释放。研究表明,土壤有机质和pH是影响土壤重金属释放潜力的重要因素,在利用植树覆绿进行重金属污染土壤改良时植树等引起的土壤有机质积累和酸化对土壤重金属释放潜力的影响应予以关注。
4通过吸附-解吸试验与培养试验等方法研究了磷灰石、农用石灰、坡缕石、钙镁磷肥、沸石和氢氧化铁6种矿物改良剂对酸性和石灰性2种污染城市土壤中重金属的固定作用及高岭石、膨润土、沸石和磷灰石4种矿物改良剂对1种Pb污染农业土壤中Pb的固定作用。吸附-解吸试验表明,磷灰石、农用石灰、坡缕石、钙镁磷肥、沸石和氢氧化铁6种矿物改良剂对Cu、Cd、Pb和Zn均有强烈的吸持作用,吸持率在97.2%以上,2次解吸后被保留在矿物上的重金属比例仍在96.8%以上。
Amacher提取法对土壤重金属的形态分析表明,2种污染城市土壤施用改良剂后,土壤中的重金属趋向稳定,交换态重金属逐渐向更稳定的形态转化,但不同改良剂的转化程度有较大差异。交换态重金属下降的程度由高至低大致为钙镁磷肥、坡缕石>氢氧化铁、沸石>农用石灰>磷灰石。施用改良剂可明显降低土壤中0.02mol·L-1CaCl_2提取的水溶性重金属,酸性土壤上施用改良剂的效果明显高于石灰性土。对于石灰性土壤,与对照相比,石灰性土壤施用改良剂后水溶性Cu、Cd、Pb、Zn分别下降了21-53%、18%-35%、22%-47%和16%-33%,酸性土壤施用改良剂后水溶性Cu、Cd、Pb、Zn分别下降了36%-68%、33-59%、41-69%、33-62%。各类改良剂在降低水溶性重金属的效果上较为相似,并以施用钙镁磷肥、坡缕石或磷灰石为佳。用上述矿物改良剂来固定Cu、Cd、Pb、Zn,降低土壤重金属的释放潜力是可行的。
加入矿物改良剂对Pb污染农业土壤易释放态Pb(水溶性Pb和交换态Pb)也有明显的降低作用,其效果与矿物类型、矿物加入量及加入矿物的磨细程度等有关。对于加Pb的处理(添加量为100mg·kg-1),培养100d后,加入高岭石、膨润土、沸石和磷灰石后土壤水溶态Pb分别比对照下降了38.11%-49.70%、64.33%-71.34%、73.48%-83.23%和83.84%-90.24%,交换态Pb分别比对照降低了25.45%-36.99%、53.29%-60.13%、64.42%-70.02%和76.19%-80.26%。矿物对Pb污染农业土壤易释放态Pb的降低作用次序为：磷灰石>沸石>膨润土>高岭石。过100目筛处理的矿物对土壤中Pb的固定效果好于过18目筛处理的矿物。加入矿物对土壤水溶性Pb的降低作用明显好于对交换态Pb的作用。利用天然矿物来改良Pb污染农业土壤可有效降低土壤Pb的释放潜力。当土壤Pb污染水平较低时,加入矿物量为20g·kg-1已能达到改良效果。
Heavy metals contamination in soils and road-deposited sediments is becoming hore and more serious while economy is developing quickly. The related problems have been focused by people. Besides transporting in soil-plant system and influencing growth of plant as well as safety of agricultural product,heavy metals in contaminated soils can also be transported to waterbody(including surface waterbody and ground waterbody) by surface runoff, leaching and so on. Water quality of waterbody and environment is influenced consequently.Soil matters can be transported and deposited on road in different ways,and heavy metals in road-deposited sediments can also be transported again to waterbody with surface runoff in proper conditions. The aim of this study was to learn about release potential, transportation law, influencing factors for the release of heavy metals in soil and road-deposited sediment,as well as methods for characterizing the release potential of heavy metals and decreasing the release potential of soil heavy metals. By analyzing samples,simulating experiment and observing in fields,potential influence on waterbody of accumulation of heavy metals in soils and road-deposited sediment was researched. Accordingly,the release and transporting law of heavy metals as well as the relation between release,tran-sporting and soil properties were researched. Furthermore,amendment methods for immobilizing heavy metals were researched. The obtained preliminary results are meaningful for assessing risk of heavy metals in soils and road-deposited sediment to waterbody as well as founding characterizing method based on water quality saftety and controlling the harm of soil heavy metals to waterbody. The main results and conclusions were:
1Sixteen paddy soils were collected and a one year indubating experiment was conducted by adding Cd and Pb to them. Release behavior of Cd and Pb in contaminated soils was assessed by determining water-soluble and exchangeable Cd and Pb. The results showed that the percentage of water-soluble and exchangeable Cd and Pb usually increased while the content of Cd and Pb in soil increased. Without adding Cd.the average percentage of water-soluble and exchangeable Cd in total Cd were0.16%and7.24%,respectively. In the treatment of adding Cd by0.2、0.5、1.0、2.0and5.0mg·kg-1,the percentage of water-soluble Cd were0.14%、0.25%、0.34%、0.50%and0.81%,respectively,and the percentage of exchangeable Cd were10.73%、11.61%、14.11%、12.55%and10.67%,respectively. Without adding Pb,the average percentage of water-soluble and exchangeable Pb were0.006、and0.70%,respect-ively. In the treatment of adding Pb by20.0,50.0、100.0、200.0and500.0mg· kg-1, the percentage of water-soluble Pb respectively were0.008%、0.014%、0.027%、0.036%and0.047%, and the percentage of exchangeable Pb were1.03%、1.71%、2.67%、3.74%and3.84%,respectively. The increasement of water-soluble and exchangeable Cd and Pb with accumulation of soil Cd and Pb varied greatly in different soils. Relation analysis showed that water-soluble Cd and Pb mainly were related with the pH and base saturation; whereas, exchangeable Cd and Pb mainly were related with pH,base saturation,CEC and texture. The increasement of water-soluble and exchangeable Cd and Pb were lower in soils with high pH,CEC,base saturation and in more clayey soils,and the release potential of Cd and Pb can be decreased more greatly in the soils. The effect of decreasing mobile speicies of Pb is bigger than that of Cd.
2Five different land-use zones (industrial, residential, commercial, park, and countryside) were selected in Hangzhou,and25road-deposited sediments were collected. The concentrations of heavy metals (Cd,Co,Cr,Cu,Fe,Mn,Ni,Pb and Zn) in these samples were determined, and chemically fractionated according to the BCR (the European Community Bureau of Reference) sequential extraction procedure. According to the enrichment factor(EF),there were anthropogenic pollution sources,concerning Cu、Cd、Pb and Zn. The high heavy metal concentration levels were detected in the samples from industrial zone and commercial zone which were influenced by heavy traffic,and so on. While the concentrations of the heavy metals were lower in the samples from residential zone,park and countryside zone. Based on the BCR sequential extration procedure Zn,Cd,Cu and Pb were more mobile and had more threat to waterbody.
In addition,sixty-three representative sites of paddy field, orchard,vege-table land, nursery and urban land in north Zhejiang plain were selected. Surf-ace runoff were collected, and water-soluble Cd,Co,Cr,Ni,Pb,Cu,Zn,Mn and Fe in the runoff samples were determined. Surface soil samples were also collected in the corresponding sites. Total heavy metals and water-soluble heavy metals were determined by extracting with0.01mol·L-1CaCl2. The results showed that the co-ncentrations of heavy metals in the runoff samples varied greatly. The water-soluble mean values for Cd、Co、Cr、Ni、Pb、Cu、Zn、Mn and Fe respectively were0.19.0.46、1.04、1.73、4.98、88.47、184.52、609.52and1135.21μg·L-1, and Cu、 Zn、Pb had bigger threat to waterbody envrionment. Land use change had an impact on the concentrations of water-soluble heavy metals in runoff samples. Maximum concentrations of Cd,Co,Cr,Ni,Pb and Zn were present in the runoff from urban area, whereas those of Mn and Fe were present in the runoff from paddy field. However, orchard land had the highest concentration Cu of runoff. The results showed that the release capacity of heavy metals is related with land use. The concentrations of water-solube heavy metals in the runoff had significantly negative correlation with pH.and significantly(or dramatically siginificantly) positive correlation with total content and water-soluble heavy metals of the corresponding soils. CaCl2-extractable heavy metals can better represent the release potential of heavy metals in surface runoff,compared with the total content. There were more heavy metals which can run off with surface runoff and threaten waterbody quality when heavy metals were concentrated in the soils, especially when mobile heavy metals were increased.
3Thirteen undisturbed soil columns in different contamination level were collected using PVC tubes. The soil columns were leached by deionized water in10mm·h-1simulating rainfall for one time. The amount of the leachate was50mm. The results showed that the percentage of water-soluble Cu, Cd, Pb and Zn in total amount were25.25%,47.52%,15.45%and35.65%, respectively. Most concentrations of water- soluble heavy metals were lower than particulate heavy metals. Water-soluble, particulate and total Cu,Cd,Pb and Zn were negatively correlated with bulk density. Water-soluble, total Cu,Cd,Pb and Zn usually were highly significant with pH. Particulate Cu,Cd,Pb and Zn were not significantly correlated with pH. Water-soluble, particulate and total Cu,Cd,Pb and Zn were negatively correlated with calcium carbonate,clay particles,organic carbon and CEC. The results indicated that soil heavy metals were leached mainly in particulate phase. Bulk density, pH,CEC,clay-particles and organic carbon were important properties which can influence leaching phase of soil heavy metals.
For researching the influence of the treatment of adding oranic material and acidifing on species and release potential of soil heavy metals,one soil samples contaminated by Cu,Cd,Pb,Zn and Cr was collected.The organic material was added in4levels:0、50、100and200g·kg-1. The acidification included control and decreasing pH to6,5,4. The soil was leached after incubating for1year. The leaching experiment was conducted for17d. The samples were leached1time every4d,and were leached5times totally. They were leached by50mm deionized water. The results showed that soil pH respectively decreased from7.1to7.0,6.8,6.8,6.7after adding0,50,100,200g·kg-1organic material without acidifing. The results indicated that accumulation of organic material can decrease soil pH slightly. The percentage of exchangeable heavy metals could increased apparently while pH decreased, especially for Cd,Zn. Pb and Cu in the leachates increased by46%-128%compared to the contol.when pH decreased to6.0,and Cd,Zn increased by219%-630%,and Cr increased by10%-119%. Cu,Cd,Pb,Zn and Cr in the leachates respectively increased by165%-555%,156%-940%,196%-475%,214%-746%and70%-444%compared to the control,when pH decreased to5.0. When pH decreased to4.0,the concentrations of heavy metals of every treatments reached to very high level. It was showed that acifification could increase acitivity and release of heavy metals. Effect of organic matter accumulation on release potential of heavy metals was related with soil pH and degree of organic matter accumulation. When pH was relatively high, low level accumulation of organic matter can increase the release of heavy metals,and high level accumulation of organic matter can decrease the release of heavy metals. However,when pH was relatively low,accumulation of organic matter can decrease the release of heavy metals. It is concluded that pH and organic matter content are important factors which influence release potential of soil heavy metals. The influence of organic materials accumulation and acidification created by afforestation when afforestation is implemented for amending contaminated soils on release potential of soil heavy metals should be concerned.
4Immobilizing effects of6mineral amendments(apatite, agricultural limestone,palysorskite,Ca-Mg-P fertilizer,zeolite and Fe(OH)3) to heavy metals in2contaminated urban soils (including a acidic soil and a calcareous soil),and4mineral amendments (kaolinite.bentonite, zeolite and apatite) to heavy metals in one Pb-contaminated agricultural soil were studied by incubating experiments, and so on. Sorption-desorption experiment showed that the6mineral amendments could strongly adsorbed Cu,Cd,Pb and Zn. The adsorption rates were more than97.2%. The6mineral amendments had strong adsorption ability for heavy metals as the remained heavy metals retained on the minerals were still more than96.8%after2times of desorption.
The Amacher sequential extraction procedure showed that the exchangeable heavy metals were gradually transformed to more stable carbonate-bound,oxide-bound and residual heavy metals after appling the6amendments,and the transformation varied with different amendments. The sequence of decrease level of exchangeable heavy metals was Ca-Mg-P fertilizer, palysorskite>Fe(OH)3, zeolite> agricultural limestone>apatite. It was showed that amendments could apparently reduce water-soluble heavy metals extracted with0.02mol·L-1CaCl2. The effect on the acidic soil was apparently better than the effect on the calcareous soil. Compared to the control,water-soluble Cu,Cd,Pb and Zn respectivley were decreased by21-53%,18%-35%,22%-47%and16%-33%,with adding amendments in the calcareous soil. Compared to the control,water-soluble Cu,Cd,Pb and Zn respectively were decreased by36%-68%、33-59%、41-69%and33-62%with adding amendments in the acidic soil. The effect for decreasing water-soluble heavy metals was best for Ca-Mg-P fertilizer,palygorskite and apatite. The amendments could apparently decrease mobility of the heavy metals. It is feasible to immobilize Cu,Cd,Pb,Zn and decrease release potential of heavy metals with the6mineral amendments.
The results showed that.adding amendments also could reduce mobile Pb (water-soluble and exchangeable Pb) in Pb-contaminated agricultural soil app-arently. The effects were related with amendments type,applied amount and the size of the amendments. In the treatment of adding Pb (added amount is100mg· kg-1), after adding kaolinite.bentonite,zeolite or apatite a-nd incubating for100d,water-soluble Pb decreased respectivley by38.11%-49.70%,64.33%-71.34%,73.48%-83.23%,83.84%-90.24%,and exchangeable Pb decreased by25.45%-36.99%,53.29%-60.13%,64.42%-70.02%,76.19%-80.26%,compared to the control. The sequence of the effects for decreasing mobile Pb in Pb-contaminated agricultural soil of the minerals was:apatite>zeolite>Bentonite>kaolinite. The immobilizing eff-ect of the minerals sieved with100#mesh was apparently better than the min-erals sieved with18#mesh. The reduction of water-soluble Pb by adding the m-inerals was bigger than the reduction of exchangeable Pb. The release potenti-al of Pb in the contaminated agricultural can be effectively decreased,by us-ing the minerals. In the contaminated soil with lower level of Pb,recommended amount of minerals for amending soil is20g·kg-1
1采集了16个稻田土壤,进行为期12个月的Cd、Pb的添加培养试验,通过测定所培养土壤中水溶态和交换态Cd、Pb评估了土壤Cd、Pb的释放行为。结果表明,随着Cd和Pb污染水平的提高,土壤中水溶态和交换态Cd和Pb占全量比例呈增加趋势。未加外源Cd时,水溶态Cd占全Cd的比例平均为0.16%,交换态Cd占全Cd的比例平均为7.24%。外源Cd加入量为0.2、0.5、1.0、2.0和5.0mg·kg-1的处理对应的土壤水溶态Cd占全Cd比例平均分别为0.14%、0.25%、0.34%、0.50%和0.81%；土壤交换态Cd占全Cd比例平均分别为10.73%、11.61%、14.11%、12.55%和10.67%。未加外源Pb时,水溶态Pb占全Pb的比例平均为0.006%,交换态Pb占全Pb的比例平均为0.70%,外源Pb加入量为20.0、50.0、100.0、200.0和500.0mg·kg-1的处理对应土壤水溶态Pb占全Pb比例平均分别为0.008%、0.014%、0.027%、0.036%和0.047%,土壤交换态Pb占全Pb比例平均分别为1.03%、1.71%、2.67%、3.74%和3.84%。不同土壤中水溶态和交换态Cd和Pb含量随土壤Cd和Pb积累的增加幅度有很大的差异。相关分析表明,土壤中水溶性Cd和Pb含量主要与土壤土壤pH、盐基饱和度有关；而交换态Cd和Pb含量主要与pH、盐基饱和度、CEC及土壤质地等有关。pH、CEC较高、质地较粘、盐基饱和度较高的土壤中水溶态、交换态Cd和Pb含量增加幅度较小,可较大程度地降低进入土壤Cd和Pb的释放潜力及对水体的威胁。土壤降低Pb易释放形态的作用高于Cd。
2在杭州选择了5种不同土地利用区(工业区、商业区、居民区、公园、农村),采集了25个道路沉积物样品,测定了样品中重金属的全量,并采用BCR提取法对重金属进行形态分级。结果表明,Cu、Cd、Pb和Zn等元素的富集因子(EF)较高,受人为来源的污染影响较大。由于受交通等污染源的影响,工业区和商业区道路沉积物中重金属含量较高,居民区、公园、农村的重金属含量较低。由BCR提取法的结果可知,道路沉积物中Zn、Cd、Cu和Pb等重金属有较大的释放潜力,对水体环境具有较大潜在威胁。
另在浙北平原选择了63个区块的代表性水田、蔬菜地、果园、苗木地和城市用地,通过收集地表径流,测定地表径流中水溶性Cu、Cd、Pb、Zn、Co、Cr、Fe、Ni、Mn的浓度,同时采集对应区块地表土壤,测定重金属含量,并用0.01mol·L-1CaCl_2溶液测定了土壤水溶态重金属含量。研究结果表明,地表径流中重金属元素平均浓度由低至高依次为Cd、Co、Cr、Ni、Pb、Cu、Zn、Mn和Fe,分别为0.19、0.46、1.04、1.73、4.98、88.47、184.52、609.52和1135.21μg·L-1, Cu、Zn和Pb对水体环境威胁相对较大。径流中Fe和Mn的浓度以水田为最高,Cu的浓度以果园为最高,Cd、Co、Cr、Ni、Pb和Zn的浓度以城区为最高,表明土壤中重金属释放强度与土地利用类型有关。地表径流中水溶性重金属浓度与土壤pH呈极显著或显著负相关,与相应土壤重金属全量和CaCl_2提取态呈极显著或显著的正相关,相比全量土壤CaCl_2提取态重金属含量更能反映土壤重金属随地表径流的流失潜力。随着土壤重金属的积累,特别是活性较高的重金属含量提高,有更多的重金属可通过地表径流流失,对水体水质会产生更大危害。
3用PVC管采集了13个具有不同污染程度的原状土柱,用去离子水进行淋溶,以10mm·h-1的速度模拟1次降雨淋溶过程,淋溶量为50mm。结果表明,淋出液中水溶态Cu、Cd、Pb和Zn占其全量的比例平均分别为25.25%、47.52%、15.45%和35.65%,大部分淋出液中水溶态重金属的浓度低于颗粒态。淋出液中水溶态、颗粒态、全量Cu、Cd、Pb、Zn浓度与土壤容重均呈负相关,水溶态、全量Cu、Cd、Pb、Zn与土壤pH一般呈极显著负相关,颗粒态Cu、Cd、Pb、Zn与pH的相关性不显著,水溶态、颗粒态、全量Cu、Cd、 Pb、Zn与土壤碳酸钙含量及土壤粘粒、有机碳含量和CEC呈负相关。土壤重金属主要以颗粒态垂直淋迁,土壤容重、pH、CEC、粘粒、有机碳是影响土壤重金属淋溶形态的重要性质。
采用受到Cu、Cd、Pb、Zn、Cr较明显污染的土壤进行了添加有机物和酸化2类处理对土壤重金属形态和释放潜力影响的研究,有机物的加入量设0、50、100和200g·kg-14个等级,酸化包括对照和使土壤pH分别降至6、5、4等4个处理,培养1午后进行淋溶试验(淋溶试验共进行17d,每4d淋溶1次,共5次,每次用100m1去离子水淋溶),并用Amacher连续提取法分析土壤重金属的形态变化。结果发现,不加酸而加入0、50、100、200g·kg1的有机物料培养后,土壤pH分别从7.1降为7.0、6.8、6.8和6.7,表明有机质的积累可使土壤pH轻微下降。pH下降可使重金属交换态比例显著增加,其中对Cd、Zn的影响最为明显。pH降至6时,淋出液中Pb、Cu比对照增加了46%-128%, Cd、Zn比对照增加了219%-630%,Cr增加了10%-119%。pH降至5时,淋出液中Cu、Cd、Pb、 Zn、Cr浓度分别比对照增加了165%-555%、156%-940%、196%-475%、214%-746%、70%-444%,pH降至4时各处理淋出液中重金属浓度都达到了很高水平。表明土壤酸化可增加重金属的活性和释放。有机质积累对重金属释放潜力的影响与pH和有机质积累程度有关,当pH较高时,低量有机质的积累可促进重金属的释放,高量有机质的积累可减少重金属的释放；而当pH较低时,有机质的积累可降低土壤重金属的释放。研究表明,土壤有机质和pH是影响土壤重金属释放潜力的重要因素,在利用植树覆绿进行重金属污染土壤改良时植树等引起的土壤有机质积累和酸化对土壤重金属释放潜力的影响应予以关注。
4通过吸附-解吸试验与培养试验等方法研究了磷灰石、农用石灰、坡缕石、钙镁磷肥、沸石和氢氧化铁6种矿物改良剂对酸性和石灰性2种污染城市土壤中重金属的固定作用及高岭石、膨润土、沸石和磷灰石4种矿物改良剂对1种Pb污染农业土壤中Pb的固定作用。吸附-解吸试验表明,磷灰石、农用石灰、坡缕石、钙镁磷肥、沸石和氢氧化铁6种矿物改良剂对Cu、Cd、Pb和Zn均有强烈的吸持作用,吸持率在97.2%以上,2次解吸后被保留在矿物上的重金属比例仍在96.8%以上。
Amacher提取法对土壤重金属的形态分析表明,2种污染城市土壤施用改良剂后,土壤中的重金属趋向稳定,交换态重金属逐渐向更稳定的形态转化,但不同改良剂的转化程度有较大差异。交换态重金属下降的程度由高至低大致为钙镁磷肥、坡缕石>氢氧化铁、沸石>农用石灰>磷灰石。施用改良剂可明显降低土壤中0.02mol·L-1CaCl_2提取的水溶性重金属,酸性土壤上施用改良剂的效果明显高于石灰性土。对于石灰性土壤,与对照相比,石灰性土壤施用改良剂后水溶性Cu、Cd、Pb、Zn分别下降了21-53%、18%-35%、22%-47%和16%-33%,酸性土壤施用改良剂后水溶性Cu、Cd、Pb、Zn分别下降了36%-68%、33-59%、41-69%、33-62%。各类改良剂在降低水溶性重金属的效果上较为相似,并以施用钙镁磷肥、坡缕石或磷灰石为佳。用上述矿物改良剂来固定Cu、Cd、Pb、Zn,降低土壤重金属的释放潜力是可行的。
加入矿物改良剂对Pb污染农业土壤易释放态Pb(水溶性Pb和交换态Pb)也有明显的降低作用,其效果与矿物类型、矿物加入量及加入矿物的磨细程度等有关。对于加Pb的处理(添加量为100mg·kg-1),培养100d后,加入高岭石、膨润土、沸石和磷灰石后土壤水溶态Pb分别比对照下降了38.11%-49.70%、64.33%-71.34%、73.48%-83.23%和83.84%-90.24%,交换态Pb分别比对照降低了25.45%-36.99%、53.29%-60.13%、64.42%-70.02%和76.19%-80.26%。矿物对Pb污染农业土壤易释放态Pb的降低作用次序为：磷灰石>沸石>膨润土>高岭石。过100目筛处理的矿物对土壤中Pb的固定效果好于过18目筛处理的矿物。加入矿物对土壤水溶性Pb的降低作用明显好于对交换态Pb的作用。利用天然矿物来改良Pb污染农业土壤可有效降低土壤Pb的释放潜力。当土壤Pb污染水平较低时,加入矿物量为20g·kg-1已能达到改良效果。
Heavy metals contamination in soils and road-deposited sediments is becoming hore and more serious while economy is developing quickly. The related problems have been focused by people. Besides transporting in soil-plant system and influencing growth of plant as well as safety of agricultural product,heavy metals in contaminated soils can also be transported to waterbody(including surface waterbody and ground waterbody) by surface runoff, leaching and so on. Water quality of waterbody and environment is influenced consequently.Soil matters can be transported and deposited on road in different ways,and heavy metals in road-deposited sediments can also be transported again to waterbody with surface runoff in proper conditions. The aim of this study was to learn about release potential, transportation law, influencing factors for the release of heavy metals in soil and road-deposited sediment,as well as methods for characterizing the release potential of heavy metals and decreasing the release potential of soil heavy metals. By analyzing samples,simulating experiment and observing in fields,potential influence on waterbody of accumulation of heavy metals in soils and road-deposited sediment was researched. Accordingly,the release and transporting law of heavy metals as well as the relation between release,tran-sporting and soil properties were researched. Furthermore,amendment methods for immobilizing heavy metals were researched. The obtained preliminary results are meaningful for assessing risk of heavy metals in soils and road-deposited sediment to waterbody as well as founding characterizing method based on water quality saftety and controlling the harm of soil heavy metals to waterbody. The main results and conclusions were:
1Sixteen paddy soils were collected and a one year indubating experiment was conducted by adding Cd and Pb to them. Release behavior of Cd and Pb in contaminated soils was assessed by determining water-soluble and exchangeable Cd and Pb. The results showed that the percentage of water-soluble and exchangeable Cd and Pb usually increased while the content of Cd and Pb in soil increased. Without adding Cd.the average percentage of water-soluble and exchangeable Cd in total Cd were0.16%and7.24%,respectively. In the treatment of adding Cd by0.2、0.5、1.0、2.0and5.0mg·kg-1,the percentage of water-soluble Cd were0.14%、0.25%、0.34%、0.50%and0.81%,respectively,and the percentage of exchangeable Cd were10.73%、11.61%、14.11%、12.55%and10.67%,respectively. Without adding Pb,the average percentage of water-soluble and exchangeable Pb were0.006、and0.70%,respect-ively. In the treatment of adding Pb by20.0,50.0、100.0、200.0and500.0mg· kg-1, the percentage of water-soluble Pb respectively were0.008%、0.014%、0.027%、0.036%and0.047%, and the percentage of exchangeable Pb were1.03%、1.71%、2.67%、3.74%and3.84%,respectively. The increasement of water-soluble and exchangeable Cd and Pb with accumulation of soil Cd and Pb varied greatly in different soils. Relation analysis showed that water-soluble Cd and Pb mainly were related with the pH and base saturation; whereas, exchangeable Cd and Pb mainly were related with pH,base saturation,CEC and texture. The increasement of water-soluble and exchangeable Cd and Pb were lower in soils with high pH,CEC,base saturation and in more clayey soils,and the release potential of Cd and Pb can be decreased more greatly in the soils. The effect of decreasing mobile speicies of Pb is bigger than that of Cd.
2Five different land-use zones (industrial, residential, commercial, park, and countryside) were selected in Hangzhou,and25road-deposited sediments were collected. The concentrations of heavy metals (Cd,Co,Cr,Cu,Fe,Mn,Ni,Pb and Zn) in these samples were determined, and chemically fractionated according to the BCR (the European Community Bureau of Reference) sequential extraction procedure. According to the enrichment factor(EF),there were anthropogenic pollution sources,concerning Cu、Cd、Pb and Zn. The high heavy metal concentration levels were detected in the samples from industrial zone and commercial zone which were influenced by heavy traffic,and so on. While the concentrations of the heavy metals were lower in the samples from residential zone,park and countryside zone. Based on the BCR sequential extration procedure Zn,Cd,Cu and Pb were more mobile and had more threat to waterbody.
In addition,sixty-three representative sites of paddy field, orchard,vege-table land, nursery and urban land in north Zhejiang plain were selected. Surf-ace runoff were collected, and water-soluble Cd,Co,Cr,Ni,Pb,Cu,Zn,Mn and Fe in the runoff samples were determined. Surface soil samples were also collected in the corresponding sites. Total heavy metals and water-soluble heavy metals were determined by extracting with0.01mol·L-1CaCl2. The results showed that the co-ncentrations of heavy metals in the runoff samples varied greatly. The water-soluble mean values for Cd、Co、Cr、Ni、Pb、Cu、Zn、Mn and Fe respectively were0.19.0.46、1.04、1.73、4.98、88.47、184.52、609.52and1135.21μg·L-1, and Cu、 Zn、Pb had bigger threat to waterbody envrionment. Land use change had an impact on the concentrations of water-soluble heavy metals in runoff samples. Maximum concentrations of Cd,Co,Cr,Ni,Pb and Zn were present in the runoff from urban area, whereas those of Mn and Fe were present in the runoff from paddy field. However, orchard land had the highest concentration Cu of runoff. The results showed that the release capacity of heavy metals is related with land use. The concentrations of water-solube heavy metals in the runoff had significantly negative correlation with pH.and significantly(or dramatically siginificantly) positive correlation with total content and water-soluble heavy metals of the corresponding soils. CaCl2-extractable heavy metals can better represent the release potential of heavy metals in surface runoff,compared with the total content. There were more heavy metals which can run off with surface runoff and threaten waterbody quality when heavy metals were concentrated in the soils, especially when mobile heavy metals were increased.
3Thirteen undisturbed soil columns in different contamination level were collected using PVC tubes. The soil columns were leached by deionized water in10mm·h-1simulating rainfall for one time. The amount of the leachate was50mm. The results showed that the percentage of water-soluble Cu, Cd, Pb and Zn in total amount were25.25%,47.52%,15.45%and35.65%, respectively. Most concentrations of water- soluble heavy metals were lower than particulate heavy metals. Water-soluble, particulate and total Cu,Cd,Pb and Zn were negatively correlated with bulk density. Water-soluble, total Cu,Cd,Pb and Zn usually were highly significant with pH. Particulate Cu,Cd,Pb and Zn were not significantly correlated with pH. Water-soluble, particulate and total Cu,Cd,Pb and Zn were negatively correlated with calcium carbonate,clay particles,organic carbon and CEC. The results indicated that soil heavy metals were leached mainly in particulate phase. Bulk density, pH,CEC,clay-particles and organic carbon were important properties which can influence leaching phase of soil heavy metals.
For researching the influence of the treatment of adding oranic material and acidifing on species and release potential of soil heavy metals,one soil samples contaminated by Cu,Cd,Pb,Zn and Cr was collected.The organic material was added in4levels:0、50、100and200g·kg-1. The acidification included control and decreasing pH to6,5,4. The soil was leached after incubating for1year. The leaching experiment was conducted for17d. The samples were leached1time every4d,and were leached5times totally. They were leached by50mm deionized water. The results showed that soil pH respectively decreased from7.1to7.0,6.8,6.8,6.7after adding0,50,100,200g·kg-1organic material without acidifing. The results indicated that accumulation of organic material can decrease soil pH slightly. The percentage of exchangeable heavy metals could increased apparently while pH decreased, especially for Cd,Zn. Pb and Cu in the leachates increased by46%-128%compared to the contol.when pH decreased to6.0,and Cd,Zn increased by219%-630%,and Cr increased by10%-119%. Cu,Cd,Pb,Zn and Cr in the leachates respectively increased by165%-555%,156%-940%,196%-475%,214%-746%and70%-444%compared to the control,when pH decreased to5.0. When pH decreased to4.0,the concentrations of heavy metals of every treatments reached to very high level. It was showed that acifification could increase acitivity and release of heavy metals. Effect of organic matter accumulation on release potential of heavy metals was related with soil pH and degree of organic matter accumulation. When pH was relatively high, low level accumulation of organic matter can increase the release of heavy metals,and high level accumulation of organic matter can decrease the release of heavy metals. However,when pH was relatively low,accumulation of organic matter can decrease the release of heavy metals. It is concluded that pH and organic matter content are important factors which influence release potential of soil heavy metals. The influence of organic materials accumulation and acidification created by afforestation when afforestation is implemented for amending contaminated soils on release potential of soil heavy metals should be concerned.
4Immobilizing effects of6mineral amendments(apatite, agricultural limestone,palysorskite,Ca-Mg-P fertilizer,zeolite and Fe(OH)3) to heavy metals in2contaminated urban soils (including a acidic soil and a calcareous soil),and4mineral amendments (kaolinite.bentonite, zeolite and apatite) to heavy metals in one Pb-contaminated agricultural soil were studied by incubating experiments, and so on. Sorption-desorption experiment showed that the6mineral amendments could strongly adsorbed Cu,Cd,Pb and Zn. The adsorption rates were more than97.2%. The6mineral amendments had strong adsorption ability for heavy metals as the remained heavy metals retained on the minerals were still more than96.8%after2times of desorption.
The Amacher sequential extraction procedure showed that the exchangeable heavy metals were gradually transformed to more stable carbonate-bound,oxide-bound and residual heavy metals after appling the6amendments,and the transformation varied with different amendments. The sequence of decrease level of exchangeable heavy metals was Ca-Mg-P fertilizer, palysorskite>Fe(OH)3, zeolite> agricultural limestone>apatite. It was showed that amendments could apparently reduce water-soluble heavy metals extracted with0.02mol·L-1CaCl2. The effect on the acidic soil was apparently better than the effect on the calcareous soil. Compared to the control,water-soluble Cu,Cd,Pb and Zn respectivley were decreased by21-53%,18%-35%,22%-47%and16%-33%,with adding amendments in the calcareous soil. Compared to the control,water-soluble Cu,Cd,Pb and Zn respectively were decreased by36%-68%、33-59%、41-69%and33-62%with adding amendments in the acidic soil. The effect for decreasing water-soluble heavy metals was best for Ca-Mg-P fertilizer,palygorskite and apatite. The amendments could apparently decrease mobility of the heavy metals. It is feasible to immobilize Cu,Cd,Pb,Zn and decrease release potential of heavy metals with the6mineral amendments.
The results showed that.adding amendments also could reduce mobile Pb (water-soluble and exchangeable Pb) in Pb-contaminated agricultural soil app-arently. The effects were related with amendments type,applied amount and the size of the amendments. In the treatment of adding Pb (added amount is100mg· kg-1), after adding kaolinite.bentonite,zeolite or apatite a-nd incubating for100d,water-soluble Pb decreased respectivley by38.11%-49.70%,64.33%-71.34%,73.48%-83.23%,83.84%-90.24%,and exchangeable Pb decreased by25.45%-36.99%,53.29%-60.13%,64.42%-70.02%,76.19%-80.26%,compared to the control. The sequence of the effects for decreasing mobile Pb in Pb-contaminated agricultural soil of the minerals was:apatite>zeolite>Bentonite>kaolinite. The immobilizing eff-ect of the minerals sieved with100#mesh was apparently better than the min-erals sieved with18#mesh. The reduction of water-soluble Pb by adding the m-inerals was bigger than the reduction of exchangeable Pb. The release potenti-al of Pb in the contaminated agricultural can be effectively decreased,by us-ing the minerals. In the contaminated soil with lower level of Pb,recommended amount of minerals for amending soil is20g·kg-1
引文
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