ISSN 1000-3665 CN 11-2202/P

    北京市平原典型区地下水硫循环过程及其对砷富集的影响

    Sulfur cycling processes and its effect on arsenic mobility in groundwater from typical areas of the Beijing Plain

    • 摘要: 北京市天然高砷(As)地下水的广泛分布显著制约了区域地下水资源的开发利用。地下水中硫(S)的循环过程是重要的水文地球化学过程之一,其如何影响地下水砷的富集尚不明确。本研究选取北京市顺义和通州区不同深度地下水开展水化学组分、\mathrmSO_4^2- 硫氧同位素及沉积物含硫矿物赋存形态的研究,旨在揭示地下水的硫循环过程对地下水砷富集的影响。研究发现:(1)高浓度As和高浓度\mathrmSO_4^2- 地下水主要分布于浅层含水层中;随着深度的增加,As和\mathrmSO_4^2- 浓度呈降低趋势;(2)地下水δ34S-SO4δ18O-SO4呈显著正相关,而与\mathrmSO_4^2- /Cl(mol/mol)呈显著负相关,表明地下水中发生了\mathrmSO_4^2- 生物还原过程。δ34S-SO4与As浓度呈正相关,而\mathrmSO_4^2- /Cl(mol/mol)与As浓度呈负相关,表明地下水中\mathrmSO_4^2- 还原促进As的释放。\mathrmSO_4^2- 还原产生的H2S驱动含砷铁氧化物的化学还原,从而导致As的释放;(3)不同深度沉积物中均检测出了较高含量的酸可挥发性硫(acid volatile sulfide, AVS)、铬还原性硫(Cr(II)-reducible sulfide, CRS)和单质硫(elemental sulfur, ES),为含水层中发生的硫循环过程及其对地下水As富集的驱动作用提供了证据。研究揭示了地下水系统中硫循环如何驱动砷的富集及转化,为S-As耦合治理地下水砷提供了理论依据。

       

      Abstract: The widespread occurrence of naturally high-arsenic (As) groundwater in Beijing severely restricts the utilization of regional groundwater resources. Sulfur cycling in groundwater is one of the important hydrogeochemical processes, yet its role in controlling As mobility remains unclear. In this study, groundwater samples from different depths in Shunyi and Tongzhou districts were analyzed for geochemical composition, sulfur and oxygen isotopes in \mathrmSO_4^2- , and the speciation of sulfur-containing minerals in sediments to reveal the influence of sulfur cycling on As enrichment in groundwater. Results suggest that high As and high \mathrmSO_4^2- groundwater are mainly enriched in shallow aquifers, with the As and \mathrmSO_4^2- concentrations gradually decreasing with depth. The positive correlation between δ34S-SO4 and δ18O-SO4, together with the increase in δ34S-SO4 with the decrease in \mathrmSO_4^2- /Cl ratio, indicates the occurrence of microbial \mathrmSO_4^2- reduction process in the groundwater. The positive correlation between δ34S-SO4 and As concentration and the negative correlation between \mathrmSO_4^2- /Cl molar ratio and As indicate that \mathrmSO_4^2- reduction promoted the release of As. The generated H2S from \mathrmSO_4^2- reduction triggered the chemical reductive dissolution of As-bearing Fe(III) oxides and the release of As. The presences of acid volatile sulfide (AVS), Cr(II)-reducible sulfide (CRS), and elemental sulfur (ES) in sediments at different depths provide evidence for the sulfur cycling process and its effect on groundwater As mobility. The study reveals how the sulfur cycling drives the enrichment and transformation of As in groundwater system, and provides theoretical basis for the coupled S-As treatment on As in groundwater.

       

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