Factors controlling mobility of 127I and 129I species in an acidic groundwater plume at the Savannah River Site

被引:73
作者
Otosaka, Shigeyoshi [1 ,2 ]
Schwehr, Kathleen A. [2 ]
Kaplan, Daniel I. [3 ]
Roberts, Kimberly A. [3 ]
Zhang, Saijin [2 ]
Xu, Chen [2 ]
Li, Hsiu-Ping [2 ]
Ho, Yi-Fang [2 ]
Brinkmeyer, Robin [2 ]
Yeager, Chris M. [3 ]
Santschi, Peter H. [2 ]
机构
[1] Japan Atom Energy Agcy, Res Grp Environm Sci, Tokai, Ibaraki 3191195, Japan
[2] Texas A&M Univ, Dept Marine Sci, Lab Oceanog & Environm Res, Galveston, TX 77553 USA
[3] Savannah River Natl Lab, Aiken, SC 29808 USA
关键词
Savannah River Site; Iodine-129; Iodine-127; Groundwater; Speciation; Iodide; Iodate; Organo-iodine; IODINE; IODATE; PLUTONIUM; CHROMATOGRAPHY; TRANSPORT; SORPTION;
D O I
10.1016/j.scitotenv.2011.05.018
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In order to quantify changes in iodine speciation and to assess factors controlling the distribution and mobility of iodine at an iodine-129 (I-129) contaminated site located at the U.S. Department of Energy's Savannah River Site (SRS), spatial distributions and transformation of I-129 and stable iodine (I-127) species in groundwater were investigated along a gradient in redox potential (654 to 360 mV), organic carbon concentration (5 to 60 mu mol L-1), and pH (pH 3.2 to 6.8). Total I-129 concentration in groundwater was 8.6 +/- 2.8 Bq L-1 immediately downstream of a former waste seepage basin (well FSB-95DR), and decreased with distance from the seepage basin. I-127 concentration decreased similarly to that of I-129. Elevated concentrations of I-127 or I-129 were not detected in groundwater collected from wells located outside of the mixed waste plume of this area. At FSB-95DR, the majority (55-86%) of iodine existed as iodide for both I-127 and I-129. Then, as the iodide move down gradient, some of it transformed into iodate and organo-iodine. Considering that iodate has a higher K-d value than iodide, we hypothesize that the production of iodate in groundwater resulted in the removal of iodine from the groundwater and consequently decreased concentrations of I-127 and I-129 in downstream areas. Significant amounts of organo-iodine species (30-82% of the total iodine) were also observed at upstream wells, including those outside the mixed waste plume. Concentrations of groundwater iodide decreased at a faster rate than organo-iodine along the transect from the seepage basin. We concluded that removal of iodine from the groundwater through the formation of high molecular weight organo-iodine species is complicated by the release of other more mobile organo-iodine species in the groundwater. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:3857 / 3865
页数:9
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