采用现代分析方法探讨零价铁(ZVI)与奥奈达希瓦氏菌(S.oneidensis)MR-1还原U(Ⅵ)的效果与机制。结果表明:ZVI与S.oneidensis均能够还原U(Ⅵ);在厌氧条件下,ZVI与S.oneidensis还原U(Ⅵ)存在协同作用。当p H为7、温度为30℃、U(Ⅵ)的初始浓度为20 mg/L、ZVI的投加量为1.0 g/L时,24 h S.oneidensis对U(Ⅵ)还原率达到96.9%;在0.5~2.0 g/L范围内,U(Ⅵ)的还原率随ZVI投量的增加而上升;在U(Ⅵ)初始浓度5.0~50.0mg/L内,U(Ⅵ)的还原率与其浓度正相关。ZVI、Fe3O4和Fe2O3均能明显促进U(Ⅵ)的还原,而可溶态的Fe(Ⅲ)对U(Ⅵ)的还原具有明显的抑制作用。其他离子Cu2+、Ca2+、Mn2+和NO3-对U(Ⅵ)的还原存在抑制作用,以Cu2+的影响最大,Ca2+的影响次之,SO42-对U(Ⅵ)的还原影响较小。XPS分析结果表明,ZVI表面吸附和沉积了U(Ⅵ)和U(Ⅳ)两种价态的U元素,反应后的铀大部分形成了稳定的UO2。
The effects and mechanism of U(Ⅵ) reduction by Shewanella oneidensis (S.oneidensis) MR-1 with zero-valent iron(ZⅥ) were evaluated. The results show that either ZⅥ or bacteria can reduce U(Ⅵ) in the solution and under anaerobic conditions, a cooperative action of ZⅥ and the bacteria S.oneidensis is observed in reducing process of U(Ⅵ). Under condition of pH 7.0, temperature 30 ℃, the initial concentration of U (Ⅵ) 20 mg/L and ZⅥ addition 1.0 g/L, the reduction rate of U(Ⅵ) reaches 96.9% by S.oneidensis reduction for 24 h. The reduction rate of U(Ⅵ) is improved with increasing amount of ZⅥ in the range of 0.5-2.0 g/L, and the reduction rate of U(Ⅵ) is positive correlated with its initial concentration in the range of 5.0-50.0 mg/L. Fe304, FeEO3 and ZⅥ are effective accelerators for bioreduction of U(Ⅵ), and soluble Fe(Ⅲ) can remarkably inhibit U(Ⅵ) bioreduction. The other coexistence ions, such as Cuz+, Ca2+, Mn2+ and NO3-, show a remarkable negative effect on U(Ⅵ) reduction, and among these ions, the negative effect of Cu2+ is the greatest and that of Ca2+ is the second. SO42- has less influence on U(Ⅵ) bioreduction. XPS results indicate the deposition of U element are in forms of U(Ⅵ) and U(IV) on iron filings surface, and the reduction product U(IV) is most likely to be in the form of UO2.