Np(Ⅴ)在漳州伊利石上吸附作用的实验及建模研究

Experimental and Modeling Study of Np(Ⅴ) Adsorption on Zhangzhou Illite

  • 摘要: 通过批吸附实验研究了固液比、pH值、离子强度和Np(Ⅴ)浓度等因素对Np(Ⅴ)在漳州伊利石上吸附作用的影响。结果表明,pH值对吸附的影响明显,而离子强度对吸附无显著影响。基于法国Puy-en-Velay伊利石的2SPNE SC/CE模型并不能拟合本研究所得的滴定数据和吸附数据。依照2SPNE SC/CE模型框架,重新构建了Np(Ⅴ)在漳州伊利石上的吸附模型。与2SPNE SC/CE模型相比,本研究所得模型的位点密度小,对应的质子转移和配位反应的平衡常数也不相同。存在这种差异的原因可能是:漳州伊利石的比表面积小于Puy-en-Velay伊利石的比表面积;Puy-en-Velay伊利石较漳州伊利石具有更高比率的同晶置换(更高的Fe2O3和MgO含量)。研究结果将有助于更准确地预测Np(Ⅴ)在不同产地伊利石上的吸附作用,为我国高放废物处置库的选址提供参考。

     

    Abstract: The adsorption of Np(Ⅴ) on Zhangzhou illite was studied as a function of solid-to-liquid ratio, pH, ionic strength and Np(Ⅴ) concentration, by using a batch experimental method. Np(Ⅴ) adsorption on Zhangzhou illite is shown to be sensitive to pH, whereas it is insensitive to ionic strength. 2SPNE SC/CE model, developed from Puy-en-Velay illite (France), cannot interpret both titration and adsorption data of Zhangzhou illite. A new adsorption model was constructed with the framework of 2SPNE SC/CE model to interpret the data. Comparing with 2SPNE SC/CE model, the site capacity of the new model is much lower, and corresponding constants of protolysis and complexation reactions are quite different as well. The reason for these differences may be due to the fact that the specific surface area of Zhangzhou illite is lower, and the ratio of isomorphous substitution (i.e. content of Fe2O3 and MgO) in Puy-en-Velay illite is higher than the one of Zhangzhou illite. The results are useful for predicting more accurately the Np(Ⅴ) adsorption on illite originated from different regions, and provide references for the siting of high-level radioactive waste repository in China.

     

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