Reduction of U(VI) by Fe(II) during the Fe(II)-Accelerated Transformation of Ferrihydrite

被引：74
作者：
Boland, Daniel D. [1 ]
Collins, Richard N. [1 ]
Glover, Chris J. [2 ]
Payne, Timothy E. [1 ,3 ]
Waite, T. David [1 ]
机构：
[1] Univ New S Wales, Sch Civil & Environm Engn, Sydney, NSW 2052, Australia
[2] Australian Synchrotron, Clayton, Vic 3168, Australia
[3] Australian Nucl Sci & Technol Org, Inst Environm Res, Kirrawee, Dc Nsw 2232, Australia
来源：
ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2014年 / 48卷 / 16期
基金：
澳大利亚研究理事会;
关键词：
OXIDE-WATER INTERFACE; FE(II)-CATALYZED TRANSFORMATION; SURFACE CATALYSIS; FLOW CONDITIONS; AQUEOUS FE(II); IRON-OXIDES; FE-II; GOETHITE; URANIUM; (OXYHYDR)OXIDES;
D O I：
10.1021/es501750z
中图分类号：
X [环境科学、安全科学];
学科分类号：
08 ; 0830 ;
摘要：
X-ray absorption spectroscopy has been used to study the reduction of adsorbed U(VI) during the Fe(II)-accelerated transformation of ferrihydrite to goethite. The fate of U(VI) was examined across a variety of pH values and Fe(II) concentrations, with results suggesting that, in all cases, it was reduced over the course of the Fe(III) phase transformation to a U(V) species incorporated in goethite. A positive correlation between U(VI) reduction and ferrihydrite transformation rate constants implies that U(VI) reduction was driven by the production of goethite under the conditions used in these studies. This interpretation was supported by additional experimental evidence that demonstrated the (fast) reduction of U(VI) to U(V) by Fe(II) in the presence of goethite only. Theoretical redox potential calculations clearly indicate that the reduction of U(VI) by Fe(II) in the presence of goethite is thermodynamically favorable. In contrast, reduction of U(VI) by Fe(II) in the presence of ferrihydrite is largely thermodynamically unfavorable within the range of conditions examined in this study.
引用
收藏
页码：9086 / 9093
页数：8
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