摘要
我国农田土地利用强度高,受人为活动影响强烈；既面临工矿企业、交通、城市化进程和公共卫生防御带来的外源污染物,又有高度集约化农业本身产生的污染,致使污染物从多渠道、多界面进入人类赖以生存的土壤环境。土壤-作物系统中呈现出“新老污染物共存、有机／无机复合污染”的复杂状况,特别是重金属和含氯持久性有机污染物造成的土壤污染已受到广泛关注。近年来不断爆发的人体、土-水环境污染事件,为污染土壤治理与修复提出了迫切的需求。本研究以重金属复合污染和重金属-有机氯农药的中轻度复合污染农田土壤为研究对象,通过新品种筛选和农艺措施调控,开展了复合污染土壤植物修复的强化技术及机制研究,取得的主要研究结果如下：
1.针对长期自然老化的重金属锌(Zn)-镉(Cd)复合污染土壤,采用盆栽土培试验研究了KH2PO4、Ca(H2PO4)2、NaH2PO4和NH4H2PO4在P205浓度为0-352mgkg-1时,一年三次连续刈割对东南景天(Sedum alfredii H.)地上部Zn、Cd积累和养分元素吸收的影响。结果表明,供试磷酸二氢盐均促进了东南景天生长,352mgP2O5kg-1显著增加了地上部干物质重；地上部磷(P)含量显著增加,Zn含量随着P浓度的增加而显著升高,而Cd含量显著下降。磷肥降低了植物地上部氮(N)、中量元素钙(Ca)、镁(Mg)、硫(S)和微量元素锰(Mn)、铁(Fe)、铜(Cu)含量,对钾(K)含量影响不显著,地上部碳(C)含量随P浓度增加而升高。植物对Zn提取量为第一茬<第二茬<第三茬,而Cd的提取量变化为第二茬<第一茬<第三茬。由于磷肥的增产效应,植物地上部对土壤Zn和Cd的提取量均显著增加,植物对重金属的最大提取量为352mg kg-1KH2PO4和NH4H2PO4处理。因此,合理磷酸盐施用能提高东南景天对Zn/Cd复合污染土壤的修复效率,缩短修复周期。
2.对盆栽土培试验土壤理化性质、微生物学指标及重金属形态分析测定发现,随着磷肥施用浓度的增加,土壤pH值显著降低(P<0.05)。较高浓度(352mg P2O5kg-1土)的四种磷肥处理时,土壤Mehlich-3提取态和可交换态及碳酸盐结合态锌含量均显著增加；而Mehlich-3提取态和交换态Cd含量显著下降,碳酸盐结合态和铁锰氧化物结合态Cd含量显著降低。磷肥施用后土壤微生物生物量碳、氮、磷显著高于对照土壤,土壤酸性磷酸酶活性在施用磷肥后显著下降(P<0.05)。东南景天地上部Zn含量与土壤Mehlich-3提取态磷含量(P<0.0001)、土壤交换态及碳酸盐结合态锌含量(P<0.001)间均存在极显著正相关关系,而与土壤pH值呈极显著负相关(P<0.0001)。该研究表明,Zn. Cd复合污染条件下,土壤施用磷肥能改变重金属形态,增加土壤锌生物有效性和超积累植物S. alfredii对锌的吸收,这是磷肥提高Zn-Cd复合污染土壤植物修复效率的重要原因。
3.通过田间条件下盆钵实验和室内分析,比较了23份优质能源作物蓖麻(Ricinus communis)不同基因型栽培种对复合污染土壤中Cd和DDTs(p,p'-DDT. o,p'-DDT、p,p'-DDD和p,p'-DDE总和,下同)的吸收和积累能力差异。结果表明,不同蓖麻品种对土壤DDTs和Cd的积累及转运能力差异较大。叶、茎、根DDTs的平均含量为0.37、0.43和70.51mg kg-1干重,Cd平均含量分别为1.22,2.27和37.63mg kg-1干重。DDTs和Cd的生物富集系数变幅分别为0.09-65.33和0.43-13.30,DDTs或Cd的转运系数均小于0.1。植物对DDTs和Cd总的积累量分别为83.06(B09032)-267.79μg(B09053),和66.04(ZJ3)-155.12μg(B09053)。较短的生长周期、高生物量、强大的根系吸收能力及其对DDTs和Cd同时积累等特性表明蓖麻作物在DDTs/Cd复合污染土壤植物修复中有很大的应用前景。
4.利用筛选到的污染物富集蓖麻品种,采用盆栽实验对比研究了零价铁粉和蓖麻联合作用对复合污染土壤的修复效果。实验结果显示：零价铁粉、非离子表面活性剂Brij35和柠檬酸等化学修复剂对植物生长均无显著影响。Brij35处理蓖麻地上部ΣDDTs含量最高,为5.79mg kg-1,显著高于Fe0和柠檬酸处理,但与对照处理差异不显著,而柠檬酸处理地上部ΣDDTs含量显著低于对照。土壤Fe0处理急剧增加了蓖麻对p,p'-DDD的吸收,含量达6.7mg kg-1干重。化学修复剂均显著降低了蓖麻地上部Cd含量,平均降幅为28.6-64.6%,Fe0和柠檬酸处理地上部Cd含量下降最为明显,显著低于Brij35处理。蓖麻种植对土壤DDTs总的提取量为144.6-193.6μg盆-1,Cd的积累量为52.78-116.28μg盆-1,其中Brij35的增加效应最为明显。种植蓖麻后土壤中ΣDDTs含量均显著下降,Fe0处理土壤ΣDDTs降解量是对照的1.85倍,而Brij35和柠檬酸处理土壤ΣDDTs降解量与对照间无显著差异。Fe0主要通过化学还原脱氯作用加速了植物修复过程中土壤DDTs降解。
5.采用室外盆栽实验研究了油茶籽饼粕(T3)、蚯蚓堆肥(T4)、生物表面活性剂茶皂素(T5)、还原硫粉(T6)对蓖麻修复DDTs-Cd复合污染土壤效率及影响机制,同时比较了接种DDT降解菌(Pseudomonas sp. DDT-1)和自然微生物条件下土壤污染物去除过程的差异。研究结果显示：外源有机废弃物添加(T3和T4)均促进了植物根系和地上部的生长,根系干物质重分别增加了22.1%和15.5%,地上部干物质重分别增加了17.4%和16.5%,但是增量不显著。土壤添加剂施用均显著降低了蓖麻地上部Cd含量,平均下降量为31.0%-45.9%；除了T4处理外,其余添加剂在一定程度上增加了蓖麻根系Cd含量,增幅为12.5%-42.5%,T5较大幅度增加了植物根系对Cd的吸收,但差异不显著。接种降解菌急剧增加了蓖麻根系Cd含量,对照处理T1增加量为8.6倍,T4处理增加量较少,为1.2倍,其它处理增幅为3.1-7.3倍。无论是自然土著微生物还是接种降解菌条件,外源施用土壤修复剂均不同程度增加了蓖麻地上部DDTs含量,最高增幅为48.0%。T3处理土壤微生物生物量碳、碱性磷酸酶、过氧化氢酶和脱氢酶活性显著高于其它处理。各修复剂处理均显著增加了土壤DDTs的降解速率,其中油茶籽饼粕(T3)处理效果最明显。综合分析认为含有生物表面活性剂成分的油茶籽饼粕废弃物是增强蓖麻修复DDTs-Cd复合污染土壤效率的适宜天然修复剂。
The use intensity of farming soil was high and it was strongly affected by human activities in our country. The soils are faced with exogenous pollutants brought by industrial and mining enterprises, traffic, urbanization process and public health defense, and also highly intensive agriculture pollution from itself. These cause pollutants from multiple sources into the soil environment for human survival. Soil-crop system was showing the complex situation as coexistence of old and new pollutants, organic and inorganic co-compounbined pollution. Especially soil pollution caused by heavy metals and chlorinated persistent organic pollutants were widespread concerned. In recent years, the constantly outbreak of environmental pollution accidents between the human body and soil-water system put forward urgent demand for contaminated soil remediation and restoration.
In this research, the screening of new energy plant varieties and agronomic measures regulation to enhance phytoremediation efficiency were carried out under the mild farmland contaminated soil with heavy metal co-contamination and heavy metal-organochlorine pesticide co-combined pollution. Through the process of phytoremediation strengthening technology and mechanism investigation, primary results were summarized as follows:
1. Improving the efficacy of phytoextraction is critical for its successful application in metal contaminated soils. Mineral nutrition affects plant growth and metal absorption and subsequently the accumulation of heavy metal through hyper-accumulator plants. This study assessed the effects of di-hydrogen phosphates (KH2PO4, Ca(H2PO4)2, NaH2P04and NH4H2PO4) application at three levels (22,88and352mg P kg-1soil) on Sedum alfredii growth and metal uptake by three consecutive harvests on aged and Zn-Cd combined contaminated paddy soil. The shoot P and Zn concentrations are enhanced significantly (P<0.05), while the Cd concentration is decreased with the increase of phosphate levels.The addition of phosphates (P) significantly increased the amount of Zn taken up by S. alfredii due to increased shoot Zn concentration and dry matter yield (DMY)(P<0.05). The phosphate application reduces N, the secondary nutrients (Ca, Mg and S) and micronutrients (Mn, Fe and Cu) concentrations, while the K concentration has no significant effect. The total carbon concentration of shoots is increased at the high P level. The amount of Zn removed by phytoextraction increased in the order of Clipping1<2nd clipping<3rd clipping, and for Cd extraction the order was2nd clipping<1st clipping<3rd clipping. The highest phytoextraction of Zn and Cd was observed in KH2PO4and NH4H2PO4treatment at352mg P kg-1soil. These results indicate that application of P fertilizers coupled with multiple cuttings can enhance the removal of Zn and Cd from contaminated soils by S. alfredii, thus shortening the time needed for accomplishing remediation goals.
2. Microcosm experiments were conducted in greenhouse to examine the effect of different phosphorus (P) sources on zinc (Zn) phytoextraction by Sedum alfredii in aged Zn contaminated paddy soil. The Zn accumulation, soil pH, microbial biomass and enzyme activity, available Zn changes and soil Zn phytoremediation efficiency after plant harvest were determined. Upon addition of P, Zn and Cd uptake of S, alfredii significantly increased. Mehlich-3extractable or the fractions of exchangeable and carbonate bound soil Zn were significantly increased at higher P applications. But Mehlich-3extractable or the fractions of exchangeable Cd significantly increased, and carbonate and Fe-Mn oxides bound Cd were significantly increased as P applications. Soil pH significantly decreased with increasing P application rates. Soil microbial biomass in the P-treated soils was significantly higher (P﹤0.05) than those in the control. Shoot Zn concentration was positively correlated with Mehlich-3extractable P (P﹤0.0001) or exchangeable/carbonate-bound Zn (P﹤0.001), but negatively related to soil pH (P﹤0.0001). These results indicate that application of P fertilizers has the potential to enhance Zn bioavaiability and uptake by hyperaccumulating plant S. alfredii, thus increasing phytoremediation efficiency of Zn contaminated soils.
3. The objective of this study was to compare the ability of23genotypes of Ricinus communis in mobilizing and uptake of Cd and DDTs (p,p'-DDT, o,p'-DDT, p,p'-DDD and p,p'-DDE) in the co-contaminated soil. The pot experiments under field conditions and laboratory analysis was done. The plant genotypes varied largely in the uptake and accumulation of DDTs and Cd, with mean concentrations of0.37,0.43and70.51for DDTs, and1.22,2.27and37.63mg kg-1dw for Cd in leaf, stem and root, respectively. The total uptake of DDTs and Cd varied from83.1(B09032) to267.8(B09053) and66.0(ZJ3) to155.1(B09053)μg per pot, respectively. These results indicate that R. communis has great potential for removing DDTs and Cd from contaminated soils attributed to its fast growth, high biomass, strong absorption and accumulation for both DDTs and Cd.
4. The pot experiment was done to evaluate the combined effecf of zero-valent iron (Fe0) and DDTs accumulating castor variety to remediate Cd and DDTs co-contaminated soil. No sgnificant (P<0.05) differences in root and shoot biomass were observed among the Fe0, nonionic surfactants Brij35and citric acid amendments. TheDTs content in castor shoot was highest under Brij35treatment with5.79mg kg-1, significantly higher than Fe0or citric acid, but no significant difference with CK; While shoot ΣDDTs content was significantly lower than CK. Fe0treatment dramaticly increase soil and plant root (6.7mg kg-1dw) p,p'-DDD content. Chemical amendments significantly decrease the shoot Cd content, an average reduction of28.6-64.6%, especially for Fe0and citric acid; they were significant lower than Brij35. The total DDTs and Cd uptake by castor were144.6-193.6μg pot-1, and52.78-116.28μg pot-1, the increase effect of the Brij35was the most obvious. Soil ΣDDTs have significantly dissipated after Fe0-castor planting; the reduction amount was1.85fold of CK, but no citric acid and Brij35treatments. Fe0abiotic dechlorination was accompanied by Ricinus communis uptake of the DDT and its intermediate metabolites such as DDE and DDD provides a promising alternative to the traditional techniques of elimination also from the economic point of view.
5. Effects of soil additives, in particular of oil tea seed residue (T3), vermicompost (T4), biosurfactant tea saponin (T5) and reduction elemental sulfur (T6) on DDTs-Cd combined soil remediation using R. communis under field pot experiment were investigated. Meanwhile, we compared the difference of DDT degradation bacteria (Pseudomonas sp. DDT-1) inoculation and indigenous microorganisms on soil pollutant removal process or plant uptake. Exogenous organic waste adding (T3/T4) improve plant root and shoot growth, the increase of root was22.1%and15.5%, and shoot was16.5-17.4%, but the increment was no significant. Soil additives singnicatly decreased shoot Cd content, an average reduction of31.0-45.9%%. Root Cd content also has some increase except for T4, T5was a substantial increase (42.5%) in the plant root Cd uptake, but the difference was not significant. Inoculation bacteria rapidly increase the castor root Cd content, the increase was8.6folds than CK, the other treatments increased by1.2-7.3folds. Whether it is indigenous microorganisms or inoculation bacteria conditions, all exogenous soil amendments increase castor shoot DDTs content, the highest increase of48.0%. The soil microbial biomass carbon, alkaline phosphatase, catalase and dehydrogenase activity of T3treatment was significantly higher than other treatments. All soil additives significantly increased the degradation rate of soil DDTs, and the most obvious effect was T3treatments. These results indicate that oil tea seed residue containing the composition of tea saponin is suitable for use on enhancing DDTs-Cd co-contaminated remediation by R. communis.
引文
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