工业场地污染土壤镉迁移过程中同位素分馏研究

Study on Isotopic Fractionation during Cadmium Migration in Contaminated Soil from Industrial Sites

  • 摘要: 镉(Cd)进入土壤后的迁移转化过程会引发不同程度的同位素分馏,因此厘清其相关分馏机制对实现Cd污染源的精准识别具有重要意义。然而,现有研究多局限于模拟土壤单一组分的静态吸附过程,缺乏对土壤复杂体系内多过程耦合Cd同位素分馏机制的探讨。本研究利用室内土柱装置,模拟酸性空白溶液(对照处理)和Cd污染溶液(Cd处理)对场地土壤的动态淋滤过程,结合Cd浓度、形态及同位素组成的分析,系统研究了Cd在土壤中的迁移转化行为及其同位素分馏特征。结果表明:在Cd处理土柱中,Cd迁移呈典型的“完全吸附–穿透–饱和”三阶段特征,该过程淋滤液的同位素组成变化幅度较大(Δ114/110Cd污染源-淋滤液= –0.32‰ ~ 0.21‰),土壤优先吸附污染源的轻Cd同位素(Δ114/110Cd土壤-淋滤液 = –0.04‰ ± 0.00‰),符合瑞利分馏规律。酸性淋滤环境下,对照土柱土壤Cd残渣态减少,Cd同位素发生显著负漂(Δ114/110Cd原土-现土 = 0.16‰),表层土壤优先释放重Cd同位素;相比之下,Cd处理土柱中的土壤Cd主要以酸提取态存在,Cd同位素呈明显正漂(Δ114/110Cd原土-现土= −0.24‰)。在忽略迁移过程分馏的前提下,采用同位素二元混合模型对土柱土壤Cd进行源解析,其结果与基于质量平衡的计算结果存在明显差异;在近污染源土层(0 ~ 5 cm)中,两者相对误差最小(RE = 0.16%),而在深层土壤中相对误差显著增大,最高可达38.02%,表明污染物迁移阶段所产生的分馏效应差异,应在实际场地的Cd同位素溯源中予以充分考虑。

     

    Abstract: The migration and transformation of cadmium (Cd) after entering the soil can induce varying degrees of isotopic fractionation. Elucidating the underlying fractionation mechanisms is crucial for the accurate identification of Cd pollution sources. However, existing studies are largely limited to static adsorption experiments simulating single soil components, and there is a paucity of research on the multi-process coupling of Cd isotopic fractionation mechanisms in complex soil systems. In this study, a laboratory soil column setup was used to simulate the dynamic leaching of site soil using an acidic blank solution (control treatment) and a Cd-contaminated solution (Cd treatment). By combining analyses of Cd concentration, speciation, and isotopic composition, the migration and transformation behavior of Cd in soil and its isotopic fractionation characteristics were systematically investigated. The results showed that Cd migration in the Cd-treated soil column exhibited typical dynamic three-stage characteristics: “Complete adsorption−Breakthrough−Saturation”. During this process, the Cd isotopic composition of the leachate exhibited significant variations (Δ114/110Cdsource-leachate = −0.32‰ to 0.21‰), and the soil preferentially adsorbed the light Cd isotopes from the pollution source (Δ114/110Cdsoil-leachate = −0.04‰ ± 0.00‰), which is consistent with Rayleigh fractionation. Under acidic leaching conditions, the residual fraction of Cd in the control soil column decreased, accompanied by a significant negative shift in the Cd isotopic composition (Δ114/110Cdoriginal soil-current soil = 0.16‰), with the surface soil preferentially releasing heavy Cd isotopes. In contrast, Cd in the Cd-treated soil column was mainly present in the acid-extractable fraction, exhibiting a clear positive shift (Δ114/110Cdoriginal soil-current soil = −0.24‰). When the fractionation effects during migration were ignored, the source apportionment of Cd in the soil column by applying the isotopic binary mixing model yielded results that differed significantly from those obtained via mass balance calculations. The relative error was minimal in the soil layer near the pollution source (0 to 5 cm, RE = 0.16%) and increased significantly with depth, reaching up to 38.02%. These findings indicate that the differential fractionation effects caused by the migration stages of pollutants should be taken into consideration in Cd isotopic source tracing at actual contaminated sites.

     

/

返回文章
返回