Determination of colloidal pyrolusite, Eu(III) and humic substance interaction: A combined batch and EXAFS approach

被引:77
作者
Sheng, Guodong [1 ,3 ]
Yang, Qi [1 ]
Peng, Feng [1 ]
Li, Hui [2 ]
Gao, Xing [4 ]
Huang, Yuying [4 ]
机构
[1] Shaoxing Univ, Coll Chem & Chem Engn, Shaoxing 312000, Zhejiang, Peoples R China
[2] Shaoxing Univ, Coll Med Sci, Shaoxing 312000, Zhejiang, Peoples R China
[3] Chinese Acad Sci, Inst Plasma Phys, Hefei 230031, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, SSRF, Shanghai 201204, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
Eu(III); Interaction mechanism; Microstructure; beta-MnO2; MANGANESE OXIDE MINERALS; METAL-ION COORDINATION; FULVIC-ACID; SORPTION; ADSORPTION; XPS; XAFS; TIME; HAUSMANNITE; BENTONITE;
D O I
10.1016/j.cej.2014.02.021
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This work determined the role of humic acid (HA) and fulvic acid (FA), which was extracted from the natural soil, in the interaction mechanism and microstructure of Eu(III) with pyrolusite (beta-MnO2) by using batch experiments and extended X-ray absorption fine structure (EXAFS) techniques. We combined macroscopic and spectroscopic approaches to see the evolution of the interaction mechanism and microstructure of Eu(III) with beta-MnO2 in the presence of HA or FA in comparation with that in the absence of HA or FA. The results suggested that Eu(III) interaction with beta-MnO2 was obviously affected by the addition of HA or FA. The interaction of Eu(III) with beta-MnO2 was enhanced at pH < 6.5 in the presence of HA or FA, while Eu(III) interaction with beta-MnO2 was reduced at pH > 6.5 in the presence of HA or FA. The EXAFS fitting results provided a molecular evidence for the findings from the batch experiments. Adsorption of HA or FA onto beta-MnO2 greatly modified the microstructure of Eu(III) onto beta-MnO2. Only binary surface complexes of Eu(III) can be formed onto beta-MnO2 in the absence of HA or FA, while both binary surface complexes and ternary surface complexes of Eu(III) can be simultaneously formed onto beta-MnO2 in the presence of HA or FA, which was mainly responsible for the enhanced Eu(III) uptake at low pH values. The results observed in this work are important for the evaluation of physicochemical behavior of long-lived radionuclides (lanthanides and actinides) in the natural soil and water environment. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:10 / 16
页数:7
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