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
相关论文
共 49 条
[41]   Temporal variation in 129I and 127I in aerosols from Xi'an, China: influence of East Asian monsoon and heavy haze events [J].
Zhang, Luyuan ;
Hou, Xiaolin ;
Xu, Sheng ;
Feng, Tian ;
Cheng, Peng ;
Fu, Yunchong ;
Chen, Ning .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2020, 20 (04) :2623-2635
[42]   Microwave-based digestion method for extraction of 127I and 129I from solid material for measurements by AMS and ICP-MS [J].
Gomez-Guzman, J. M. ;
Enamorado-Baez, S. M. ;
Pinto-Gomez, A. R. ;
Abril-Hernandez, J. M. .
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY, 2011, 303 (2-3) :103-108
[43]   Determination of 129I and 127I Concentration in Soil Samples from the Chernobyl 30-km Zone by AMS and ICP-MS [J].
Sahoo, Sarata Kumar ;
Muramatsu, Yasuyuki ;
Yoshida, Satoshi ;
Matsuzaki, Hiroyuki ;
Ruehm, Werner .
JOURNAL OF RADIATION RESEARCH, 2009, 50 (04) :325-332
[44]   Comparison of stable isotopes, ratios of 36Cl/Cl and 129I/127I in brine and deep groundwater from the Pacific coastal region and the eastern margin of the Japan Sea [J].
Mahara, Yasunori ;
Ohta, Tomoko ;
Tokunaga, Tomochika ;
Matsuzaki, Hiroyuki ;
Nakata, Eiji ;
Miyamoto, Yuki ;
Mizuochi, Yukihiro ;
Tashiro, Toshiharu ;
Ono, Masahiro ;
Igarashi, Toshifumi ;
Nagao, Keisuke .
APPLIED GEOCHEMISTRY, 2012, 27 (12) :2389-2402
[45]   Determination of 129I/127I in environmental water before and after the 2011 Fukushima Daiichi nuclear power plant accident with a solid extraction disk [J].
Bamba, Shigeru ;
Yamaguchi, Kosei E. ;
Amano, Hikaru .
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY, 2014, 301 (01) :75-80
[46]   Pore-water mobility: Distribution of δ37Cl, 36Cl/Cl, 129I/127I and dissolved 4He concentration in the core drilled in the Mobara gas field, Japan [J].
Mahara, Yasunori ;
Ohta, Tomoko ;
Tokunaga, Tomochika ;
Matsuzaki, Hiroyuki ;
Nagao, Keisuke ;
Nakata, Eiji ;
Miyamoto, Yuki ;
Kubota, Takumi .
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS, 2013, 294 :597-601
[47]   A Novel Approach for the Simultaneous Determination of Iodide, Iodate and Organo-Iodide for 127I and 129I in Environmental Samples Using Gas Chromatography-Mass Spectrometry [J].
Zhang, S. ;
Schwehr, K. A. ;
Ho, Y. -F. ;
Xu, C. ;
Roberts, K. A. ;
Kaplan, D. I. ;
Brinkmeyer, R. ;
Yeager, C. M. ;
Santschi, P. H. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (23) :9042-9048
[48]   Iodide Accumulation by Aerobic Bacteria Isolated from Subsurface Sediments of a 129I-Contaminated Aquifer at the Savannah River Site, South Carolina [J].
Li, Hsiu-Ping ;
Brinkmeyer, Robin ;
Jones, Whitney L. ;
Zhang, Saijin ;
Xu, Chen ;
Schwehr, Kathy A. ;
Santschi, Peter H. ;
Kaplan, Daniel I. ;
Yeager, Chris M. .
APPLIED AND ENVIRONMENTAL MICROBIOLOGY, 2011, 77 (06) :2153-2160
[49]   129I/127I and Δ14C records in a modern coral from Rowley Shoals off northwestern Australia reflect the 20th-century human nuclear activities and ocean/atmosphere circulations [J].
Mitsuguchi, Takehiro ;
Okabe, Nobuaki ;
Yokoyama, Yusuke ;
Yoneda, Minoru ;
Shibata, Yasuyuki ;
Fujita, Natsuko ;
Watanabe, Takahiro ;
Saito-Kokubu, Yoko .
JOURNAL OF ENVIRONMENTAL RADIOACTIVITY, 2021, 235