A single-site reactive transport model of Cs+ for the in situ diffusion and retention (DR) experiment

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• 作者：Shuping Yi ; Javier Samper ; Acacia Naves ; Josep M. Soler
• 关键词：Radionuclide diffusion ; Reactive transport model ; Cation exchange ; Cs+ ; In situ diffusion and retention test ; Opalinus clay ; Switzerland
• 刊名：Environmental Earth Sciences
• 出版年：2015
• 出版时间：August 2015
• 年：2015
• 卷：74
• 期：4
• 页码：3589-3601
• 全文大小：2,075 KB
• 参考文献：Appelo CAJ, Postma D (1993) Geochemistry, groundwater and pollution. Balkema, Rotterdam, pp 536
  Appelo CAJ, Van Loon LR, Wersin P (2010) Multicomponent diffusion of a suite of tracers (HTO, Cl, Br, I, Na, Sr, Cs) in a single simple of Opalinus Clay. Geochim Cosmochim Acta 74:1201-219View Article
  Atun G, Bodur N (2002) Retention of Cs on zeolite, bentonite and their mixtures. J Radioanal Nucl Chem 253(2):275-79View Article
  Atun G, Kilislioglu A (2003) Adsorption behavior of cesium on montmorillonite-type clay in the presence of potassium ions. J Radioanal Nucl Chem 258(3):605-11View Article
  Bradbury MH, Baeyens B (2000) A generalised sorption model for the concentration dependent uptake of caesium by argillaceous rocks. J Contam Hydrol 42:141-63View Article
  Dai Z, Samper J (2006) Inverse modeling of water flow and multicomponent reactive transport in coastal aquifer systems. J Hydrol 327:447-61View Article
  Dai Z, Samper J, Ritzi R (2006) Identifying geochemical processes by inverse modeling of multicomponent reactive transport in Aquia aquifer. Geosphere 4:210-19View Article
  Dai Z, Wolfsberg A, Lu Z, Deng H (2009) Scale dependence of sorption coefficients for contaminant transport in saturated fractured rock. Geophys Res Lett 36:L01403. doi:10.-029/-008GL036516 View Article
  Dai Z, Wolfsberg A, Reimus P, Deng H, Kwicklis E, Ding M, Ware D, Ye M (2012) Identification of sorption processes and parameters for radionuclide transport in fractured rock. J Hydrol 414-15:516-26
  Dewonck S (2007) Expérimentation DIR. Synthese des résultats obtenus au 01/03/07. Laboratoire de recherche souterrain de Meuse/Haute-Marne. ANDRA report D.RP.ALS.07-0044
  Gaines LG, Thomas CH (1953) Adsorption studies on clay minerals. II. A formulation of the thermodynamics of exchange adsorption. J Chem Phys 21:714-18View Article
  García-Gutiérrez M, Missana T, Mingarro M, Samper J, Dai Z, Molinero J (2001) Solute transport properties of compacted Ca-bentonite used in FEBEX Project. J Contam Hydrol 47(3):127-37View Article
  Gimmi T (2006) DR experiment Mont Terri: compilation of input data for calculations. Technical note of the DR project. Mont Terri Project, Switzerland
  Gimmi T, Leupin O, Eikenberg J, Glaus M, Van Loon LR, Waber N, Wersin P, Wang H, Grolimund D, Borca CN, Dewonck S, Wittebrood C (2014) Anisotropic diffusion at the field scale in a 4-year multi-tracer diffusion and retention experiment—I: insights from the experimental data. Geochim Cosmochim Acta 125(2014):373-93. doi:10.-016/?j.?gca.-013.-0.-14 View Article
  Gutiérrez M, Fuentes HR (1996) A mechanistic modeling of montmorillonite contamination by cesium sorption. Appl Clay Sci 11:11-4View Article
  Jakob A, Pfingstein W, Van Loon L (2009) Effects of sorption competition on caesium diffusion through compacted argillaceous rock. Geochim Cosmochim Acta 73:2441-456View Article
  Jan YL, Tsai SC, Jan JC, Hsu CN (2006) Additivity of the distribution ratio of Cs and Se on bentonite/quartz sand mixture in seawater. J Radioanal Nucl Chem 267(1):225-31View Article
  Khan SA (2003) Sorption of the long-lived radionuclides cesium-134, strotium-85 and cobalt-60 on bentonite. J Radioanal Nucl Chem 258(1):3-View Article
  Klika Z, Kraus L, Vopalka D (2007) Cesium uptake from aqueous solutions by bentonite: a comparison of multicomponent sorption with ion-exchange models. Langmuir 23:1227-233View Article
  Lauber M, Baeyens B, Bradbury MH (2000) Physico-chemical characterization and sorption measurements of Cs, Sr, ni, Eu, Th, Sn and Se on Opalinus Clay from Mont Terri. PSI technical report 00-10. Also in: Nagra tecnnical report NTB 00-11
  Lu C, Samper J, Fritz B, Clement A, Montenegro L (2011) Interactions of corrosion products and bentonite: an extended multicomponent reactive transport model. Phys Chem Earth Parts A/B/C 36:1661-668. doi:10.-016/?j.?pce.-011.-7.-13 View Article
  Molinero J, Samper J (2006) Modeling of reactive solute transport in fracture zones of granitic bedrocks. J Contam Hydrol 82:293-18View Article
  Molinero J, Samper J, Yang C, Zhang G (2004) Biogeochemical reactive transport model of the Redox zone experiment of the ?sp? hard rock laboratory (Sweden). Nucl Technol 48(2):151-65
  Montavon G, Alhajji E, Grambow B (2006) Study of the interaction of Ni2+ and Cs+ on MX-80 bentonite: effect of compaction using the “Capillary method- Environ Sci Technol 40:4672-679View Article
  Murali MS, Mathur JN (2002) Sorption characteristics of Am(III), Sr(II) and Cs(I) on bentonite and granite. J Radioanal Nucl Chem 254(1):129-36View Article
  Naves A, Samper J, Gimmi T (2012) Identifiability of diffusion and sorption parameters from in situ diffusion experiments by using simultaneously tracer dilution and claystone data. J Contam Hydrol 142-43(2012):63-4. doi:10.-016/?j.?jconhyd.-012.-9.-05 View Article
  Palut JM, Montarnal P, Gautschi A, Tevissen E, Mouche E (2003) C
• 作者单位：Shuping Yi (1) (2)
  Javier Samper (2)
  Acacia Naves (2)
  Josep M. Soler (3)
  
  1. Electric Power Design Institute, China Energy Engineering Group Co., Ltd., 510663, Guangzhou, China
  2. Escuela de Ingenieros de Caminos. Universidad de A Coru?a, Campus de Elvi?a, 15192, A Coru?a, Spain
  3. IDAEA-CSIC, 08034, Barcelona, Spain
  
• 刊物类别：Earth and Environmental Science
• 刊物主题：None Assigned
• 出版者：Springer Berlin Heidelberg
• ISSN：1866-6299

文摘

In situ diffusion experiments are performed in underground research laboratories for understanding and quantifying radionuclide diffusion from underground radioactive waste repositories. The in situ diffusion and retention, DR, experiment was performed at the Mont Terri underground research laboratory, Switzerland, to characterize the diffusion and retention parameters of the Opalinus clay. Several tracers were injected instantaneously in the circulating artificial water and were then allowed to diffuse into the clay rock through two porous packed-off sections of a borehole drilled normal to the bedding of the clay formation. This paper presents a single-site multicomponent reactive transport model of Cs+, a tracer used in the DR experiment which sorbs onto Opalinus clay via cation exchange. The reactive transport model accounts for the diffusive-reactive transport of 11 primary species and 22 aqueous complexes, and the water–rock interactions for 5 cation exchange and 3 mineral dissolution/precipitation reactions. Most of the solutes except for Cs+ diffuse from the Opalinus clay formation into the injection interval because the concentrations in the initial Opalinus clay pore water are larger than those of the initial water in the circulation system. Calcite dissolves near the borehole while dolomite precipitates. Dissolved Cs+ sorbs by exchanging with Ca2+ in the exchange complex. The computed dilution curve of Cs+ in the circulating fluid is most sensitive to the effective diffusion, D e, of the filter, the selectivity coefficient of Na+ to Cs+, K Na–Cs and D e of the borehole disturbed zone. The apparent distribution coefficient of Cs+, \(K_{\text{d}}^{\text{a}}\), in the formation varies in space and time from 100 to 165 L/kg due to the temporal changes in the water chemistry in the formation. The results of a sensitivity run in which the initial chemical composition of the Opalinus pore water is the same as the initial chemical composition of the water in the circulation system show that the changes in \(K_{\text{d}}^{\text{a}}\) are negligible. The dilution curve of Cs+ computed with the reactive transport model coincides with that obtained with the K d model. The tracer concentrations along the overcoring profiles computed with the K d model, however, differ significantly from those computed with the reactive transport model. Therefore, a reactive transport model is needed for the appropriate interpretation of the Cs+ overcoring data from the DR diffusion experiment.