摘要
本文以赤泥为研究对象,通过在重金属污染稻田土壤上开展土壤培养试验、盆栽试验和田间试验,研究赤泥对重金属的吸附特征及钝化机理,探讨重金属在水稻植株-土壤系统中迁移及输入输出特性,揭示赤泥在钝化土壤潜在毒性元素中的行为与效果,阐明赤泥的肥效机制及其对水稻和土壤环境的作用机理和效果,提出赤泥在重金属污染稻田土壤上的适宜施用量,为赤泥在农业生产上安全、有效的应用提供理论依据。主要研究结果如下：
施赤泥能显著降低土壤中交换态Pb、Zn和Cd含量,当赤泥用量为4%(W/W)时,培养30d、60 d和90 d后,交换态Pb含量分别比不施赤泥的对照处理下降了39.25%、41.38%和50.19%；交换态Zn含量分别比对照处理下降了49.26%、57.32%和47.16%；交换态Cd含量分别比对照处理下降了19.53%、24.06%和25.70%。赤泥对土壤的修复作用机理是赤泥对土壤中的重金属离子Pb2+、Zn2+和Cd2+等有较好的固着性能,使其从可交换状态转变为键合氧化物状态,从而使土壤中重金属离子的活动性和反应性降低。施用赤泥对土壤Pb、Zn和Cd五种形态所占总Pb、Zn和Cd的比重有明显影响,添加不同赤泥处理均降低了土壤中交换态Pb、Zn和Cd占总Pb、Zn和Cd的比重,且土壤中交换态Pb、Zn和Cd占总Pb、Zn和Cd的比重随赤泥施用量的增加而下降。
施用赤泥、石灰和海泡石均能有效促进土壤交换态Cd稳定化,有利于重金属Cd的固定,但三种改良剂中以赤泥的Cd钝化效果最佳。与石灰、海泡石相比,施入赤泥处理土壤中可交换态Cd分别降低了1.81%和3.55%,糙米中镉含量分别下降了17.39%和26.32%。三种改良剂中施用赤泥的增产幅度较大,施用海泡石略有增产,施用石灰的处理产量略有下降。施用改良剂能增加水稻的气孔导度(Gs)、净光合速率(Pn)、胞间CO2浓度(Ci)及蒸腾速率(Tr),其中以施赤泥处理效果较明显。各改良剂处理剑叶面积均有不同程度的上升。与石灰和海泡石相比,添加赤泥更能起到缓解Cd对水稻生长的影响,降低Cd对水稻的伤害。
在Pb、Zn和Cd严重污染的中性矿区土壤上,施用低量的0.25%(W/W)赤泥能促进水稻植株的生长和稻谷产量的增加。稻谷产量随赤泥施用量的增加呈先增加后下降的变化趋势,施0.25%(W/W)、0.5%(W/W)、0.75%(W/W)处理的稻谷产量较未施赤泥处理提高了12.04%、6.25%和4.40%；1.0%(W/W)和1.25%(W/W)处理较未施赤泥处理降低了0.23%和8.10%。施赤泥对降低作物体内Pb、Zn和Cd的含量有明显效果,以赤泥施用量较高的1.25%(W/W)处理效果最好,降幅分别达33.77%、9.84%和15.40%,但糙米中的Pb和Cd的含量仍未达食品卫生标准(Pb 0.4 mg/kg, GB14935-1994; Cd 0.2mg/kg,GB15201-95),锌含量低于50 mg/kg,达到食品卫生标准(Zn 50mg/kg,GB13106-1991)。Pb在水稻植株中的富集系数表现为：根>茎叶>壳>糙米,Zn和Cd在水稻植株中的富集系数表现为：根>茎叶>糙米>壳,且随着赤泥施用量的增加,水稻重金属Pb、Zn和Cd的富集能力降低。三种重金属的迁移能力由高到低的顺序为Cd>Zn>Pb。
施适宜用量赤泥能促进水稻植株生长和稻谷产量增加；提高土壤pH和阳离子交换量,改善土壤微生物生存环境,促进土壤细菌、真菌、放线菌生长繁殖,增加土壤微生物量C (SMBC)、微生物量N (SMBN)含量；并能提高分蘖期土壤脲酶、酸性磷酸酶和过氧化氢酶的活性；但对有机质含量的影响不明显。其中,黄泥田上0.5%(W/W)赤泥施用量较其它施用量更有利于改善Cd污染水稻土生物学性状,提高土壤肥力,而潮泥田上为0.75%(W/W)赤泥施用量较适宜。施用赤泥能提高土壤pH,降低土壤交换态Cd含量,将交换态Cd转变为铁锰结合态和碳酸盐结合态,减少水稻糙米中Cd的累积量。当赤泥施用量达到或高于0.5%(W/W)时,两种土壤上水稻的糙米Cd含量达到国家粮食卫生标准。综合考虑水稻产量、土壤修复效应和糙米品质,黄泥田和潮泥田污染土壤上的推荐赤泥施用量分别为0.5%(W/W)和0.75%(W/W)。
在中轻度Cd污染的酸性潮泥田上,稻谷产量随赤泥施用量的增加均呈先增加后下降的变化趋势。早稻以施4500 kg/hm2赤泥的最高,晚稻以施3000 kg/hm2赤泥的最高,分别比不施赤泥处理增加了11.36%和8.30%；早、晚稻水稻株高、有效穗和千粒重随赤泥施用量的增加均呈先增加后下降的变化趋势；而穗总粒随赤泥施用量的增加呈先下降后增加的变化趋势。水稻生长各时期土壤pH值随赤泥施用量的增加均有不同程度的提高,施用赤泥后土壤有效态Cd含量减少是土壤pH升高与土壤吸附能力增强共同作用的结果。水稻吸收累积Cd随赤泥施用量的增加而降低,其主要原因是施用赤泥后土壤有效态Cd含量减少。
水稻产量在一定赤泥／猪粪比施用量范围内增加,但超过一定施用量后反而有所下降。早、晚稻水稻株高、有效穗、结实率和千粒重的变化趋势与稻谷产量的变化趋势基本一致；随着赤泥／猪粪比的增加,早、晚稻土壤有效态Cd含量逐渐降低。赤泥与猪粪配施可维持叶片中超氧化物岐化酶(SOD)和过氧化物酶(POD)的较高生理活性,降低丙二醛(MDA)在叶片中的积累,改善细胞内活性氧产生与清除之间的平衡关系。随着赤泥／猪粪比的增大,水稻糙米中镉含量逐渐减少。赤泥与猪粪配施对重金属Cd污染土壤的改良效应,存在一个最适配比(早稻,1.125；晚稻,0.625)的问题,并不是越多越好。
Absorption characteristics and passivation mechanism of red mud to heavy metals in contaminated paddy soil were studied through batch, pot and field experiments. I explored the characteristics of migration, input and output of heavy metals in soil-rice plant system, and revealed the behavior and efficiency of the red mud in passivation of the potential toxic elements in the soil. I also clarified the fertilizer efficiency of red mud and its impacts on the rice plant and soil environment. I also recommended the optimum amount of red mud application to provide a theoretic basis for the safe and effective application of red mud in agricultural production. The main results were as the follows:
Application of red mud reduced soil exchangeable Pb, Zn and Cd content significantly. In comparison with the control, exchangeable Pb content was decreased by 39.25%, 41.38% and 50.19%, exchangeable Zn content was decreased by 49.26%,57.32% and 47.16%, and exchangeable Cd content was decreased by 19.53%,24.06% and 25.70% respectively after 30 d,60 d and 90 d of application of 4%(W/W) red mud. The remediation mechanism is that red mud has good fixing capacity on heavy metal ions such as Pb2+, Zn2+and Cd2+, which make them transformed from exchangeable state into a bonding oxide state. Consequently, mobility and reactivity of heavy metal ions in the soil were decreased. Application of red mud reduced the proportion of five forms of Pb, Zn and Cd, and reduced the proportion of soil exchangeable Pb, Zn and Cd to total Pb, Zn and Cd. Furthermore, the proportion of exchangeable Pb, Zn and Cd to total Pb, Zn and Cd decreased with the increasing amount of red mud application.
Application of red mud, lime and sepiolite effectively promoted the stabilization of soil exchangeable Cd. Among them, the effect of red mud was the best. Compared with lime and sepiolite treatment, soil exchangeable Cd in the red mud treatment was decreased by 1.81% and 3.55% respectively, and Cd content in brown rice was decreased by 17.39% and 26.32% respectively. Among the three soil amendments, application of red mud can increase production dramatically, while lime and sepiolite application have no apparent effects on production. Application of soil amendments increased rice stomatal conductance (Gs), the net photosynthetic rate (Pn), intercellular CO2 concentration (Ci) and transpiration rate (Tr). Among them, the effect of application of red mud disposal is obvious. Each soil amendment increased the flag leaf area variously. Compared with lime and sepiolite, red mud application could alleviate the effect of Cd on rice growth and decrease Cd damage on rice plant.
In Pb-, Zn- and Cd-polluted neutral mine soils, application of 0.25%(W/W) of red mud can promote the growth of rice plants and increase rice yield. Grain yield increased with increasing red mud application and then decreased. Compared with treatment without red mud application, grain yield increased by 12.04%,6.25% and 4.40% in treatments applied 0.25% (W/W),0.5% (W/W) and 0.75%(W/W) red mud respectively; decreased by 0.23% and 8.10% in treatments with 1% (W/W) and 1.25% (W/W) red mud application respectively. Application of red mud could significantly reduce Pb, Zn and Cd contents in rice plant, and the treatment with 1.25% (W/W) red mud application performed best, in which Pb, Zn and Cd contents reduced by 33.77%,9.84% and 15.40% respectively. Zinc content was below 50 mg/kg, which reached food hygiene standards (Zn 50 mg/kg, GB13106-1991). However, the Pb and Cd content in brown rice did not meet the food hygiene standards (Pb 0.4 mg/kg, GB14935-1994; Cd 0.2mg/kg, GB15201-95). Enrichment coefficients of Zn and Cd in rice plant were:root>stem and leaf>brown>shell, while Pb was root>stem and leaf>shell>brown. The enrichment capacity of rice plant on Pb, Zn and Cd reduced with the increasing application of red mud. Migration capacities of three heavy metals were:Cd>Zn>Pb.
The appropriate application of red mud can apparently promote rice growth and increase rice yield. With increasing amount of red mud application, soil pH value and cation exchange capacity (CEC) increased. It can be concluded that the appropriate application of red mud can improve soil microbial survival environment, promote the reproduction of soil bacteria, fungi and actinomycetes, increase the soil microbial biomass carbon (SMBC) and nitrogen (SMBN) content, and improve soil urease, acid phosphatase and catalase activity at the tillering stage, whereas the influence of red bud application on the organic content is not obvious. For the yellow clayey paddy soil,0.5% (W/W) red mud application is more beneficial to improve the soil biological characteristics and soil fertility. For alluvial loamy paddy soil,0.75%(W/W) red mud application is optimum. The application of red mud can increased soil pH, reduce the content of soil exchangeable Cd, transform exchangeable Cd into iron manganese bound and carbonate bound, and reduce the cumulative amount of Cd in brown rice. When the amount of red mud application reached or was higher than 0.5%(W/W), Cd content in brown rice in two kinds of soil meet the national food hygiene standards. Considering the type of rice yield, the effect soil remediation and the quality of brown rice, the recommended amount of red mud application on the yellow clayey paddy soil and alluvial loamy paddy soil 1 were 0.5%(W/W) and 0.75%(W/W), respectively.
In the Cd moderately contaminated acidity alluvial loamy paddy soil, grain yield increased with increasing red mud application and then decreased. In early rice, the yield in treatment with 4500 kg/hm2 red mud is highest. In late rice, the yield in treatment with 3000 kg/hm2 of red mud is highest. The grain yield in early rice and late rice was increased by 11.36% and 8.30%, respectively. Plant height, effective panicle number and 1000-grain weight in early rice and late rice were increased first and then decreased with increasing red mud application. Total grains in a particle decreased first and then increased with increasing red mud application. Soil pH value increased variably with increasing application of red mud during the stage of rice growth. Reduction of soil available Cd content was the combined results of increased soil pH value and soil adsorption capacity. The accumulation of Cd in rice decreased with increasing amount of red mud application. The primary reason is that soil available Cd content reduced after application of red mud.
Grain yield increased within a range of red mud and pig manure ratio, but the yield decreased when beyond the upper limit amount of red mud. The changing trend of plant height, effective panicle, filled grain percent and 1000-grain weight is almost the same as the trend of grain yield in early rice and late rice. With red mud and pig manure ratio increases, soil available Cd content decreased gradually in early rice and late rice. The red mud-pig manure mixer can maintain higher physiological activity of superoxide dismutase (SOD) and peroxidase (POD) in blades, decreased the accumulation malondialdehyde (MDA) in leaves, and improved the balance relationship between generation and the clearance of intracellular reactive oxygen. With the red mud to pig manure ratio increases, the contents of cadmium in brown rice decreased gradually. The effect of red mud and pig manure on improvement of Cd-contaminated soil exists an optimal ratio (early rice,1.125; late rice,0.625), rather than the more the better.
引文
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