Development of JAEA Sorption Database (JAEA …Figure 3.3-3 Overview of sorption data for selenium on granitic rocks .....43 Figure 3.3-4 Overview of sorption data for technetium on

JAEA-Data/Code

2015-028

DOI:10.11484/jaea-data-code-2015-028

日本原子力研究開発機構

March 2016

Japan Atomic Energy Agency

Yukio TACHI and Tadahiro SUYAMA

Development of JAEA Sorption Database ( JAEA-SDB) :

Update of Sorption/QA Data in FY2015

Radioactive Waste Processing and Disposal Research DepartmentNuclear Backend Technology Center

Nuclear Fuel Cycle Engineering LaboratoriesSector of Decommissioning and Radioactive Waste Management

本レポートは国立研究開発法人日本原子力研究開発機構が不定期に発行する成果報告書です。

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なお、本レポートの全文は日本原子力研究開発機構ホームページ（http://www.jaea.go.jp）より発信されています。

This report is issued irregularly by Japan Atomic Energy Agency.Inquiries about availability and/or copyright of this report should be addressed toInstitutional Repository Section,Intellectual Resources Management and R&D Collaboration Department,Japan Atomic Energy Agency.2-4 Shirakata, Tokai-mura, Naka-gun, Ibaraki-ken 319-1195 JapanTel +81-29-282-6387, Fax +81-29-282-5920, E-mail:[email protected]

© Japan Atomic Energy Agency, 2016

国立研究開発法人日本原子力研究開発機構研究連携成果展開部研究成果管理課

〒319-1195 茨城県那珂郡東海村大字白方 2 番地4電話 029-282-6387, Fax 029-282-5920, E-mail:[email protected]

JAEA-Data/Code 2015-028

Development of JAEA Sorption Database (JAEA-SDB) :

Update of Sorption/QA Data in FY2015

Yukio TACHI and Tadahiro SUYAMA※

Radioactive Waste Processing and Disposal Research Department, Nuclear Backend Technology Center, Nuclear Fuel Cycle Engineering Laboratories,

Sector of Decommissioning and Radioactive Waste Management Japan Atomic Energy Agency

Tokai-mura, Naka-gun, Ibaraki-ken

（Received December 18, 2015）

Sorption and diffusion of radionuclides in buffer materials (bentonite) and rocks are the key processes

in the safe geological disposal of radioactive waste, because migration of radionuclides in these barrier materials is expected to be diffusion-controlled and retarded by sorption processes. It is therefore necessary to understand the sorption and diffusion processes and develop databases compiling reliable data and mechanistic/predictive models, so that reliable parameters can be set under a variety of geochemical conditions relevant to performance assessment (PA).

For this purpose, Japan Atomic Energy Agency (JAEA) has developed databases of sorption and diffusion parameters in bentonites and rocks. These sorption and diffusion databases (SDB/DDB) were firstly developed as an important basis for the H12 PA of high-level radioactive waste disposal, and have been provided through the Web. JAEA has been continuing to improve and update the SDB/DDB in view of potential future data needs, focusing on assuring the desired quality level and testing the usefulness of the databases for possible applications to PA-related parameter setting.

The present report focuses on improving and updating of the sorption database (JAEA-SDB) as basis of integrated approach for PA-related Kd setting and mechanistic sorption model development. This includes an overview of database structure, contents and functions including additional data evaluation function focusing on statistical data evaluation and grouping of data related to potential perturbations. Kd data and their QA results are updated by focusing our recent activities on the Kd setting and mechanistic model development. As a result, 11,206 Kd data from 83 references were added, total number of Kd values in the JAEA-SDB reached about 58,000. The QA/classified Kd data reached about 60% for all Kd data in JAEA-SDB. The updated JAEA-SDB is expected to make it possible to obtain quick overview of the available data, and to have suitable access to the respective data for PA-related Kd setting in effective, traceable and transparent manner.

Keywords: Database, Sorption, Kd, Bentonite, Rock, Parameter Setting, Geological Disposal ―――――――――――――――――――――――――――――――――――――――― ※ Collaborating Engineer

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JAEA 収着データベース(JAEA-SDB)の開発：

2015 年度における収着データ/信頼度情報の拡充

日本原子力研究開発機構

バックエンド研究開発部門核燃料サイクル工学研究所環境技術開発センター

基盤技術研究開発部

舘幸男，陶山忠宏※

（2015 年 12 月 18 日受理）

放射性廃棄物地層処分の性能評価において，放射性核種の緩衝材（ベントナイト）及び岩石

中での収着・拡散現象は，その移行遅延を支配する重要な現象である。これら収着・拡散現象

の理解，信頼性の高い収着・拡散データを集約したデータベース，並びに現象論的モデル/評価手法の開発が，性能評価において，様々な地球化学条件を考慮して信頼性の高い核種移行パラ

メータ設定を行う上で重要となる。この目的のために，日本原子力研究開発機構では，ベントナイト及び岩石を対象として，収

着・拡散パラメータに関するデータベース開発を進めている。これら収着・拡散データベース

（SDB/DDB）は，第 2 次取りまとめを契機として最初のデータベースを整備し，ホームページでの公開を進めてきた。さらに，今後の性能評価におけるニーズへの対応を念頭に，データベ

ースに含まれるデータの信頼度評価，実際の地質環境に対するパラメータ設定におけるデータ

ベース適用等に着目して，データベースの改良・更新を継続的に実施してきた。本報告は，性能評価における Kd 設定のための統合的手法の構築の基礎として，収着データベ

ース（JAEA-SDB）の改良と更新の現状について報告する。はじめに JAEA-SDB の開発の現状として，データベースの構造と内容，今回拡充した統計評価や擾乱影響に関するデータの分類

を含む機能等の概要をまとめる。Kd データと信頼度情報の更新については，Kd 設定や現象論モデル開発との関連に着目して実施した。今回の更新において，83 の文献から 11,206 件の Kdデータとその信頼度情報が追加され，JAEA-SDB に含まれる Kd データは約 58,000 件となり，全データのうちの約 60%のデータに対して信頼度情報が付与されたこととなる。今回更新されたJAEA-SDB によって，収着データベースから利用可能な関連データ群の速やかな抽出，Kd 設定の際に参照すべきデータの適切な選定が，一層の効率性，追跡性，透明性をもって可能となる

と考えられる。

―――――――――――――――――――――――――――――――――――――――― 核燃料サイクル工学研究所 : 〒319-1194 茨城県那珂郡東海村村松 4-33 ※ 技術開発協力員

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Contents 1. Introduction ............................................................................................................................................. 1 2. Overview of JAEA-SDB and additional data evaluation functions ........................................................ 3

2.1 System, functions and contents of JAEA-SDB .......................................................................... 3 2.1.1 Overview and status of JAEA-SDB ............................................................................ 3 2.1.2 Main data table and contents of JAEA-SDB ................................................................. 4 2.1.3 Scheme and Criteria for QA/classification of Kd in JAEA-SDB ................................... 5

2.2 Additional functions for data evaluation .................................................................................... 7 2.2.1 Function of statistical data evaluation ........................................................................ 7 2.2.2 Function of grouping for Kd data related to the potential perturbations ........................ 9

3. Updating of sorption data and its QA classification .............................................................................. 10 3.1 Selection of sorption data to be included in JAEA-SDB ............................................................. 10 3.2 QA evaluation on Criteria-I and -II.............................................................................................. 22 3.3 QA evaluation on Criteria III ....................................................................................................... 41

3.3.1 Evaluation of data for trivalent of actinide and lanthanide .......................................... 41 3.3.2 Evaluation of data for radium and strontium ............................................................... 42 3.3.3 Evaluation of data for selenium ................................................................................... 42 3.3.4 Evaluation of data for technetium................................................................................ 43 3.3.5 Evaluation of data for tetravalent of actinide............................................................... 44

4. Conclusions ........................................................................................................................................... 45 Acknowledgement .................................................................................................................................... 45 References ................................................................................................................................................. 46 Appendix : QA/classification guideline for JAEA-SDB ........................................................................... 49


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目次

1. はじめに ................................................................................................................................................. 1

2. 拡充された機能を含む JAEA-SDB の概要と性能評価への適用 .................................................... 3 2.1 JAEA-SDB のシステム，機能，内容 ........................................................................................ 3 2.1.1 JAEA-SDB の概要と現状 ............................................................................................ 3 2.1.2 JAEA-SDB のメインデータテーブルと内容 ............................................................ 4 2.1.3 JAEA-SDB の Kd の信頼度評価と分類の方法と基準 .............................................. 5 2.2 データ評価のための追加機能 ................................................................................................... 7 2.2.1 統計的データ評価の機能 ............................................................................................ 7 2.2.2 潜在的擾乱影響に関する Kd データの分類の機能 .................................................. 9

3. 収着データとその信頼度情報の更新 ............................................................................................... 10 3.1 JAEA-SDB に追加する収着データの選定 .............................................................................. 10 3.2 基準 I と II に関する信頼度評価 ............................................................................................. 22 3.3 基準 III に関する信頼度評価 ................................................................................................... 41 3.3.1 3 価のアクチニドおよびランタニドの評価 ........................................................... 41 3.3.2 ラジウムおよびストロンチウムの評価 .................................................................. 42 3.3.3 セレンの評価 .............................................................................................................. 42 3.3.4 テクネチウムの評価 .................................................................................................. 43 3.3.5 4 価のアクチニドの評価 ........................................................................................... 44

4. 結論 ....................................................................................................................................................... 45

謝辞 ........................................................................................................................................................... 45

参考文献 ................................................................................................................................................... 46

付録 : JAEA-SDB の信頼度評価ガイドライン .................................................................................... 49


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Figure Contents Figure 1.1 Integrated approach for sorption/diffusion parameter setting for PA ........................................ 2 Figure 2.1 Additional functions of statistical data evaluation ................................................................... 8 Figure 2.2 Additional functions of grouping for Kd data related to the potential perturbations ................. 9 Figure 3.3-1 Overview of sorption data for trivalent of actinide and lanthanide on granitic rocks .......... 41 Figure 3.3-2 Overview of sorption data for radium and strontium on granitic rocks................................ 42 Figure 3.3-3 Overview of sorption data for selenium on granitic rocks ................................................... 43 Figure 3.3-4 Overview of sorption data for technetium on granitic rocks ................................................ 43 Figure 3.3-5 Overview of sorption data for tetravalent of actinide on granitic rocks ............................... 44

Table Contents Table 2.1 Summary of contents, functions, and systems of JAEA-SDB system and content ..................... 3 Table 2.2 Main data table of JAEA-SDB .................................................................................................... 4 Table 2.3 Reliability information table of Sorption Database (JAEA-SDB) .............................................. 6 Table 3.1 Overview of 83 references selected for updating the JAEA-SDB ............................................ 11 Table 3.2 Overview of references additionally evaluated the QA............................................................. 29


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1. Introduction

Sorption and diffusion of radionuclides in buffer materials (bentonite) and host rocks (rock matrix) are the key processes in the safe geological disposal of radioactive waste, because migration of radionuclides in these barrier materials is expected to be diffusion-controlled and retarded by sorption processes. Sorption and diffusion of radionuclides on these barrier materials depends critically on relevant geochemical conditions, especially Kd values are highly conditional parameters1),2). It is therefore necessary to understand the detailed/coupled processes of diffusion and sorption in compacted bentonite/intact rock, and to develop the database containing extensive compilation of sorption Kd data and the mechanistic/predictive model/database, so that reliable parameters can be set under a variety of geochemical conditions relevant to performance assessment (PA).

Japan Atomic Energy Agency (JAEA) has developed the sorption database (SDB), which were firstly developed as an important basis for the H12 performance assessment3),4). JAEA has been and is continuing to improve and update the SDB in view of potential future data needs, focusing on;

1) updating of sorption data5)-8)

2) assuring the desired quality level for SDB7),9)-12)

3) testing and applying of the SDB to parameter-setting13)-17).

The web-based sorption database system (JAEA-SDB) has been developed to utilize quality assuring procedure and to allow effective application for parameter setting18)( www//migrationdb.jaea.go.jp).

JAEA has developed the integrated approaches for site-specific Kd setting for PA calculations, as shown in Figure 1.1, can be made available by three different approaches;

1) experimental data acquisition for specific/reference conditions

2) extraction and conversion from existing sorption and diffusion data through SDB/DDB

3) prediction by mechanistic sorption and diffusion model

Because of the conditional nature of sorption data, Kd values to be used in PA calculations need to correspond to the specific conditions that characterize the respective PA-setting. In addition, geochemical variability or uncertainty, and their effect on Kd, usually have to be considered for reference and alternative scenarios in PA, as discussed in NEA1). Since it is not feasible to measure Kd values for all PA conditions, the use of existing sorption data obtained under generic experimental conditions and transferring such data to a range of PA-specific conditions is therefore a key challenge. The sorption database (SDB), containing large amount of sorption data for approximated, simplified, or generic systems, are used to Kd setting for PA conditions by taking into account any differences in substrate and geochemical conditions. This transfer can be done through expert judgment and semi-quantitative way, by considering difference in e.g. surface sites, speciations, competitive reactions, etc.1),13),14),17),19),20). The thermodynamic sorption model (TSM) makes it possible to estimate Kd variations directly, based on mechanistic understanding, as shown in NEA1). JAEA has developed the integrated sorption/diffusion (ISD) database in combination with thermodynamic sorption and diffusion model, and tested to explain the sorption and diffusion behavior of various radionuclides with a complex chemistry in compacted bentonites21)-23). JAEA has also tested these Kd setting approach for the derivation of Kd values and their uncertainties for rock matrix such as Horonobe

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mudstones and generic granites13)-17).

Figure 1.1 Integrated approach for sorption/diffusion parameter setting for PA

The present report focuses on updating of the sorption database (JAEA-SDB) as basis of integrated Kd setting approach shown in Figure 1.1. This includes an overview of basic functions and structures of the web-based JAEA-SDB, including updated functions to effective data evaluation (Chapter 2), updating of Kd data and QA classification, related to Kd-setting and TSM development (Chapter 3).

Geochemical conditions Repository concepts/designs

Uncertainty factors

Kd/De dataset for PA(including estimation of the associated uncertainties)

Mechanistic ModelExperimental DataAcquisition

Implementorand regulator

needs

Stepwise disposal program

- Compilation of Measured Kd/De

- QA/classification- Conversion method

by scaling factor

- Standard experimental method

- In-situ and intact system

Sorption/DiffusionDatabase

- Thermodynamic sorption model and database

- Spectroscopic evidences (EXAFS etc.)

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2. Overview of JAEA-SDB and additional data evaluation functions

2.1 System, functions and contents of JAEA-SDB

2.1.1 Overview and status of JAEA-SDB

The JAEA-SDB is a compilation of original Kd data for key radionuclides sorption on bentonite buffer, various rocks, cementitious materials and soils related to the radioactive waste disposal, determined by batch sorption experiments, including Kd values and associated experimental information. It is implemented in database software that allows quick searching/plotting of data as a function of selected key parameters. The contents, functions and systems are briefly summarized in Table 2.1. As pointed out in NEA sorption database project1), the sorption database cannot be used blindly in PA-related Kd setting, without understanding and checking carefully the experimental details, because SDB includes a great variety of Kd obtained under various conditions and with different reliability levels. The JAEA-SDB has been therefore developed by focusing the following points, so that reliable and respective data relevant to PA conditions can be extracted from SDB in effective way;

1) detailed experimental conditions to understand and check the method and conditions (see 2.1.2) 2) QA/classification scheme to check the reliability (see 2.1.3) 3) database functions to focusing on multi-parametric and statistical evaluation of Kd (see 2.2.1)

Table 2.1 Summary of contents, functions, and systems of JAEA-SDB system and content

Contents/functions Brief description for status Number of Kd values / references

Kd ; 57,875 (11,206 was added in this update*) Reference ; 699 (83 references were added in this update*)

Elements 78 elements; 1st group (related to HLW disposal); Ac, Am, Bi, Cm, Cs, Nb, Ni, Np, Pa, Pb,

Pd, Po, Pu, Ra, Sb, Se, Sm, Sn, Tc, Th, U, Zr 2nd group; Ag, Ba, Ca, Ce, Cl, Co, Eu, Fe, I, Mn, Mo, Na, Nd, Ru, Sr, Zn Minor group; 40 elements

Solid phase Bentonite (clay minerals); Rocks – 5 group; Basaltic rock, Granitic rock, Mudstone, Sandstone, Tuff; Other minerals (Fe, Al-oxides/hydroxide, calcite, etc.); Cementitious materials (cement / concrete); Soils; Having special influence (grout, organic substance etc.)*

Search parameters Element, Solid phase group Detailed – solid phase, water type, pH, Eh, ionic strength, Temperature,

solid/liquid ratio, contact time, initial concentration, separation method, atmosphere/redox condition

Graphing/data evaluation

Kd plot as a function of ; pH, Eh, ionic strength, temperature, solid/liquid ratio, contact time, initial concentration;

Grouping function to evaluate multi-parameter dependence; Statistical data evaluation*; Grouping of Kd data related to perturbations*

QA/classification QA information evaluated by QA guideline, and related evidences 34,421 Kd (about 60% of total Kd) for key RNs on Bentonite*, Mudstone, Granitic rock*, Tuff have been evaluated

Database systems - Web application based database (since 2009) - Microsoft AccessⓇ database (since 2003 / stand-alone / limited functions)

*; Contents and functions updated in this report.

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2.1.2 Main data table and contents of JAEA-SDB

Main data table of JAEA-SDB contains Kd values and a large number of additional key information describing the experimental conditions and procedures pertinent to each Kd value associated, such as solid phase properties, solution composition and pH, radionuclide redox state and initial concentration, solid/liquid ratio, and reference information, etc., as shown in Table 2.2. The hierarchical structure comprising of primary and detailed information is used to allow effective database operations.

Table 2.2 Main data table of JAEA-SDB (1/2)

Category Parameters and notes recorded Unit Remarks No. Save No. - Number for managing data record

elements Element - chemical symbol (basic search condition) Redox - valence of

Solid phase

Solid Phase Group - Solid phase group (basic search condition)

Solid Phase - Name of solid phase as rocks, clay minerals, minerals, etc.

Detailed Info.

Specific Surface Area m2/g CEC meq/100g Cation Exchange Capacity Chemical/mineral composition mm as PDF file

Note - Particle size, Source, Name, conditions and methods for sample preparation, etc.

Liquid / Solid ratio

Liquid/Solid mL/g Liquid to Solid ratio Detailed Info.

Liquid mL Amount of liquid phase Solid g Amount of solid phase

Liquid phase

water type - Type and name of solution/groundwater

Detailed Info.

Ca ppm Final or initial composition (concentration) Na ppm K ppm Mg ppm Cl ppm HCO3 ppm HCO3- + CO32- SO4 ppm F ppm SiO2 ppm Fe ppm NO3 ppm ClO4 ppm Ionic strength mol/L Calculated from each ion concentration Doc ppm Concentration of dissolved organic carbon

note - Details of type, name and preparation methods for test solution pH init - Initial pH pH end - Final pH Eh init mV Initial Eh Eh end mV Final Eh

Experimental condition

atm./redox condition - Atmosphere, Reducing agent, etc. C init mol/L Initial concentration of nuclide temp degC

Contact time day Separation - Solid-liquid separation method

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Table 2.2 Main data table of JAEA-SDB (2/2)

Category Parameters and notes recorded Unit Remarks

Distribution coefficient

Kd m3/kg Distribution coefficient

Detailed Info.

error m3/kg Error

type of information - type of Kd value reported, such as table, graph plot, etc. replicates, n - Replicate numbers of experiments

Literature

Reference - Reference as source of data

Detailed Info.

Author - Year - Title - Journal - Publisher - Vol - No - Page -

Note - Additional information on related reference such as detailed report

Others additional Information - Additional explanation related to measurement of distribution coefficient

2.1.3 Scheme and Criteria for QA/classification of Kd in JAEA-SDB

As described in 2.1.1, it is important to assess the reliability of a wide variety of Kd data in SDB for PA-related Kd setting. The reliability of Kd values in the JAEA-SDB has been assessed using the following three main criteria;

Criteria I) Completeness of documentation and type of Kd information: - the documentation of each entry is detailed enough to allow further examination in the Criteria II. - the reliability of Kd data input ; available in table format in comparison to graph format.

Criteria II) Quality of reported data: - the appropriateness of the experimental conditions and procedures to produce reliable Kd data from a

technical and scientific point of view. Criteria III) Consistency of data:

- the examination of the level of internal consistency in SDB by comparing other Kd values in similar systems.

The QA/classification guideline describing details of each Criteria and overall classification scheme is shown in Appendix9), and is briefly summarized in Table 2.3.

According to the guideline, Criteria I and key checkpoints II-b, II-c, II-d, II-h in Criteria II were evaluated first. Classification and final numerical rating were only completed when an entry was evaluated as reliable based on these checkpoints. Otherwise, entries were labeled "unreliable" and were excluded from further evaluation. The three Criteria I-III are evaluated separately, the all results can be referred in JAEA-SDB7). The JAEA-SDB uses the QA level (class I-VI), classified according to the total sum of points obtained for Criteria II, and the result of “unreliable” evaluation in Criteria I and II, as main reliability information. All results and evidences of Criteria I and II are also recorded in tabular form, can be referred as PDF format in JAEA-SDB to keep the traceability. The results pertaining to Criteria III are discussed subsequently and are illustrated in the form of plots of Kd vs. a relevant master variable (typically pH), can be referred as PDF format in JAEA-SDB.

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Table 2.3 Reliability information table of Sorption Database (JAEA-SDB)

QA-Criteria / checkpoints Brief description

SDB parameters related Rating

Criteria I) Completeness of documentation and type of Kd information:

I-a.1 Completeness of information Completeness of key parameter fields as screening for further classification

Key parameters as marked * below Yes/No

I-a.2 Information of units Completeness of units for Kd data etc. Kd, same as above Yes/No

I-b Type of Kd information Classification of level depending on Table/Figure, Kd/%-sorbed, linear/log

type of information class 1-6

Criteria II) Quality of reported data: Rating Weighting factor

II-a Solid phase Sufficient characterization of solid phase ; major minerals, impurities, surface characteristic

solid phase, specific surface area, CEC

A, B, C/D ×2

II-b* Adjustment and control of pH* Appropriate control of pH by acid-base and pH buffers pH init, pH end A, B, C, D ×8

II-c* Redox conditions* Appropriate control of redox condition, reducing agent

atm./redox condition, redox A/B, C/D ×8

II-d* Final solution composition* composition from direct measurements of thermodynamic calculations

solution composition A/B, C/D ×8

II-e Temperature Control to keep constant temperature Temperature A/B, C/D ×1

II-f Liquid/Solid ratio and particle size

Surface area of solid phase, weight of solid phase to avoid influence by vessel walls

solution/solid, specific surface area

A/B, C/D ×2

II-g Sorption value Appropriate experimental design to avoid sorption values near 0 % and 100 %

Kd, solution/solid A, B, C/D ×2

II-h* Initial RN concentration*

Confirmation of initial concentration setting less than solubility limit. (Calculation and experimental result under similar condition is applied)

C init, Solution Composition, pH A, B, C/D ×8

II-i* Phase separation* Appropriate phase separation method Separation A, B, C/D ×8

II-j* Reaction time* Confirmation for equilibrium by kinetic experiments, reasonably long reaction time

contact time A/B, C/D ×2

II-k Agitation method Appropriate agitation method - A/B, C/D ×1

II-l RN loading Appropriate RN loading to keep linear sorption, isotherm measurement

solution/solid, C init, A, B, C/D ×2

II-m Reaction vessels Appropriate material for vessels, correction by blank tests, etc. - A, B, C/D ×1

II-n Uncertainty estimates Uncertainties based repeated experiments, error propagation error, replicates (n) A, B, C, D ×2

II-o Parameter variation Systematic variations of key parameters

C init, pH init, pH end, solution/solid A, B, C, D ×8

Criteria III) Consistency of data:

III

Evaluation of Kd reliability from the perspective of consistency among data* When there is clear mismatching with Kd of another similar experimental condition and the reason is not explained, the case is classified as unreliable.

Kd reliable, unreliable

*; indicates critical checkpoints with minimum requirements related with the judgment to be ‘unreliable’.

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2.2 Additional functions for data evaluation

The main objective of JAEA-SDB is to search of Kd data for related systems and to investigate Kd trends by plotting as a function of selected key parameters. These functions can be implemented in database software that allows quick searching/plotting of data as a wide variety of function of key parameters. Main functions and operating steps are i) searching, ii) viewing datasheet, iii) graph plotting, and iv) data download as shown in details in the previous report7). In addition to data evaluating functions developed until the previous update7), two functions were added;

i) Function of statistical data evaluation to support PA-related Kd and uncertainty setting

ii) Function of grouping for Kd data related to the potential perturbations.

2.2.1 Function of statistical data evaluation

A typical challenge is the relatively limited amount of site-specific data can be made available, due to experimental constraint and complexity of conditions. The sorption database (SDB), containing large amount of sorption data for approximated, simplified, or generic systems, are therefore expected to play a central role in PA-related Kd setting.

The JAEA-SDB has been applied and tested for PA-related Kd setting by using the data evaluation functions including QA/classification and multi-parameter dependence, etc (as shown in the previous report7)). Kd data are conditional parameter, depending on various conditions such as pH, ionic strength, initial concentration of radionuclides, etc. Kd data in JAEA-SDB can be searched by ‘elements’, ‘solid phase group’ and key parameters such as pH/Eh, ionic strength and initial concentration of radionuclides, solid/liquid ratio, and then can be extracted based on QA/classification results according to Criteria I-III. Kd plotting as a function of geochemical condition such as pH usually shows a wide variation in Kd values as a result of various parameter dependence. PA-related Kd setting needs to access to the respective Kd data correspond to the specific PA conditions from a wide variety of Kd in the SDB. The data evaluation function focusing on multi-parameter dependence makes it possible to extract such dataset by investigating multi-parameter dependence between various key parameters7). The Kd distribution can be finally confirmed as histogram graph, and the Kd values and their uncertainty range need to be set for the performance assessment.

In the derivation of the Kd values and their uncertainty range, it is important to select appropriate statistical treatments by considering Kd distributions. For this purpose, functions of statistical data evaluation were additionally introduced to JAEA-SDB. Two types of representative treatments for Kd setting were selected and introduced based on previous PA-related parameter setting and related discussions for uncertainty treatment24)-26): i) median values and 95/5 percentiles, ii) log mean values and standard deviations. As shown in Figure 2.1, these statistical treatments can support the setting of the Kd values and their uncertainty range.

- 7 -


Figure 2.1 Additional functions of statistical data evaluation

Kd(m3/kg)

- 8 -


2.2.2 Function of grouping for Kd data related to the potential perturbations

Kd data are conditional parameter, depending on various conditions such as pH, ionic strength, initial concentration of radionuclides, etc. Kd plotting as a function of pH usually shows a wide variation in Kd values as a result of various parameter dependence. PA-related Kd setting needs to access to the respective Kd data correspond to the specific PA conditions from a wide variety of Kd in the SDB. For this purpose, data evaluation function focusing on multi-parameter dependence has been introduced in the JAEA-SDB7). This function makes it possible to investigate multi-parameter dependence between various key parameters.

In addition to the analysis of Kd variations corresponding to geochemical conditions, the effect of coexisting competitive ligands must be considered in developing and using the sorption database. Natural and synthetic organics can cause significant effects on sorption of radionuclides. Natural groundwaters typically contain dissolved organic substances such as humic and fulvic acids. As synthetic organic and inorganic ligands27), low-molecular-weight organics (e.g., EDTA) resulted in degradation of organic materials, and isosaccharinic acid resulted in degradation of cellulose, as well as concrete admixtures (e.g., water reducers and superplasticizers)28) are taken into account as potential perturbations. Possible impacts of these perturbations on radionuclides sorption have been considered and quantified as reduction factors29). For this purpose, the function for grouping the Kd data related to the potential perturbations as shown in Figure 2.2.

Figure 2.2 Additional functions of grouping for Kd data related to the potential perturbations

Added FA or HA

- 9 -


3. Updating of sorption data and its QA classification

3.1 Selection of sorption data to be included in JAEA-SDB

As above mentioned, the sorption database plays important roles in PA-related Kd setting and mechanistic sorption model development. In this update, the references are therefore selected in relation to our recent activities on the mechanistic model/database development22),23) and PA-related Kd setting14)-17). Primary systems focused in this updating are key radionuclides in i) montmorillonite/bentonite, ii) other clay minerals in relation to modeling and Kd setting for argillaceous and granitic rocks, and iii) new data for various barrier materials such as cement from the published literature. Selected 83 references are listed as following, and their systems are summarized in Table 3.1.

- 10 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(1/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

1)

A

dele

ye e

t al.(

1994

) A

dele

ye, S

. A. ,

Cla

y, P

. G. a

nd O

ladi

po, M

. O. A

. : S

orpt

ion

of

cesi

um, s

tront

ium

and

eur

opiu

m io

ns o

n cl

ay m

iner

als,

Jour

nal o

f M

ater

ials

Sci

ence

, vol

.29,

pp.

954-

958

(199

4).

Cs,

Eu, S

r N

a-m

ontm

orill

onite

, kao

linite

, N

a-ka

olin

ite,

Ca-

mon

tmor

illon

ite,

Ca-

kaol

inite

dist

illed

wat

er

2)

Aky

il et

al.(

1998

) A

kyil,

S. ,

Asl

ani,

M. A

. A. a

nd A

ytas

, S. :

Dis

tribu

tion

of u

rani

um

on z

eolit

e X

and

inve

stig

atio

n of

ther

mod

ynam

ic p

aram

eter

s for

th

is s

yste

m, J

ourn

al o

f Allo

ys a

nd C

ompo

unds

, vol

.271

/273

, pp

.769

-776

(199

8).

U

zeol

ite

U so

lutio

n

3)

And

erss

on e

t al

.(200

8)

And

erss

on, M

. , E

rvan

ne, H

. , G

laus

, M. A

. , H

olge

rsso

n, S

. ,

Kar

ttune

n, P

. , L

aine

, H. ,

Lot

henb

ach,

B. ,

Pui

gdom

enec

h, I.

, Sc

hwyn

, B. ,

Sne

llman

, M. ,

Ued

a, H

. , V

uorio

, M. ,

Wie

land

, E.

and

Yam

amot

o, T

. : D

evel

opm

ent o

f Met

hodo

logy

for E

valu

atio

n of

Lo

ng-te

rm S

afel

y A

spec

ts o

f Org

anic

Cem

ent P

aste

Com

pone

nts,

POSI

VA W

orki

ng R

epor

t, 20

08-2

8 (2

008)

.

Eu, N

i, Th

gr

anite

, gra

nite

_inc

l.SP,

cem

ent

past

e_in

cl.S

P ar

tific

ial c

emen

t pas

te

pore

w

ater

, gro

ut

leac

hing

Olk

iluot

o Sa

line

Wat

er, O

lkilu

oto

Salin

e W

ater

, gro

ut

leac

hing

wat

er

4)

Atu

n an

d B

odur

(200

2)

Atu

n, G

. and

Bod

ur, N

. : R

eten

tion

of C

s on

zeol

ite, b

ento

nite

and

th

eir m

ixtu

res,

Jour

nal o

f Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try,

vol.2

53, N

o.2,

pp.

275-

279

(200

2).

Cs

bent

onite

, zeo

lite

0.00

05M

, 0.0

05M

, 0.

05M

, 0.5

M, 1

M N

aCl

5)

Bor

tun

et a

l.(19

98)

Bor

tun,

A. I

. , B

ortu

n, L

. N. ,

Kha

inak

ov, S

. A. a

nd C

lear

field

, A. :

Io

n ex

chan

ge p

rope

rties

of t

he so

dium

phl

ogop

ite a

nd b

iotit

e,

Solv

ent E

xtra

ctio

n an

d Io

n Ex

chan

ge, v

ol.1

6, N

o.4,

pp.

1067

-109

0 (1

998)

.

Ba,

Ca,

C

d, C

o,

Cs,

Cu,

H

g, K

, Li,

Mg,

Pb,

R

b, S

r, Zn

Na-

biot

ite, N

a-ph

logo

pite

0.

0005

M-1

M N

aNO

3, 0.

01M

-1M

CaC

l 2,

0.01

M-0

.5M

HN

O3,

1-3M

NaO

H, B

aCl 2,

C

aCl 2,

CdC

l 2, C

oCl 2,

C

sCl,

CuC

l 2, H

gCl 2,

K

Cl,

LiC

l, M

gCl 2,

Pb

Cl 2,

RbC

l, Sr

Cl 2,

Zn

Cl 2,

gro

undw

ater

, 1M

NaN

O3+

(0

.001

M-1

M)N

aOH

6)

B

radb

ury

and

Bae

yens

(200

6)

Bra

dbur

y, M

. H. a

nd B

aeye

ns, B

. : M

odel

ling

sorp

tion

data

for t

he

actin

ides

Am

(III

), N

p(V

) and

Pa(

V) o

n m

ontm

orill

onite

, R

adio

chim

ica A

cta,

vol

.94,

pp.

619-

625

(200

6).

Am

, Eu,

N

p, P

a C

a-m

ontm

orill

onite

, N

a-m

ontm

orill

onite

0.

01M

, 0.1

M N

aClO

4, 0.

066M

CaC

l 2

- 11 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(2/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

7)

B

radb

ury

and

Bae

yens

(201

1)

Bra

dbur

y, M

. H. a

nd B

aeye

ns, B

. : P

hysi

co-C

hem

ical

C

hara

cter

isat

ion

Dat

a an

d So

rptio

n M

easu

rem

ents

of C

s, N

i, Eu

, Th

, U, C

l, I a

nd S

e on

MX

-80

Ben

toni

te, P

SI R

epor

t, PS

I Ber

icht

N

r. 11

-05

(201

1).

Cs,

Eu, I

, N

i, Se

, Th,

U

MX

-80

Pore

wat

er

8)

Che

n an

d D

ong(

2013

) C

hen,

L. a

nd D

ong,

Y. :

Sor

ptio

n of

63N

i(II)

to m

ontm

orill

onite

as a

fu

nctio

n of

pH

, ion

ic st

reng

th, f

orei

gn io

ns a

nd h

umic

subs

tanc

es,

Jour

nal o

f Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try, v

ol.2

95,

pp.2

117-

2123

(201

3).

Ni

mon

tmor

illon

ite,

mon

tmor

illon

ite+H

A

0.00

1M-0

.1M

N

aClO

4, 0.

01M

K

ClO

4, 0.

01M

Li

ClO

4, 0.

01M

NaC

l, 0.

01M

NaN

O3

9)

Del

Ner

o et

al.(

1997

) D

el N

ero,

M. ,

Mad

e, B

. , B

onte

ms,

G. a

nd C

lem

ent,

A. :

A

dsor

ptio

n of

nep

tuni

um(V

) on

hydr

argi

llite

, Rad

ioch

imic

a A

cta,

vo

l.76,

pp.

219-

228

(199

7).

Np

hydr

argi

llite

0.

001M

-0.1

M

NaC

lO4

10)

Del

Ner

o et

al.(

1998

) D

el N

ero,

M. ,

Ben

Sai

d, K

. , M

ade,

B. ,

Cle

men

t, A

. and

Bon

tem

s, G

. : E

ffect

of p

H a

nd c

arbo

nate

con

cent

ratio

n in

solu

tion

on th

e so

rptio

n of

nep

tuni

um(V

) by

hydr

argi

llite

: App

licat

ion

of th

e no

n-el

ectro

stat

ic m

odel

, Rad

ioch

imic

a A

cta,

vol

.81,

pp.

133-

141

(199

8).

Np

hydr

argi

llite

0.

1M N

aClO

4, 0.

1M

NaC

lO4+

NaH

CO

3

11)

Don

g et

al.(

2011

) D

ong,

Y. ,

Liu

, Z. a

nd L

i, Y.

: Ef

fect

of p

H, i

onic

stre

ngth

, for

eign

io

ns a

nd h

umic

subs

tanc

e on

Th(

IV) s

orpt

ion

to

GM

Z be

nton

ite

stud

ied

by b

atch

exp

erim

ents

, Jou

rnal

of R

adio

anal

ytic

al a

nd

Nuc

lear

Che

mis

try, v

ol.2

89, p

p.25

7-26

5 (2

011)

.

Th

GM

Z be

nton

ite, N

a-be

nton

ite

0.00

1M-0

.1M

N

aNO

3, 0.

01M

NaC

l, 0.

01M

KN

O3,

0.01

M

LiN

O3

12)

El-R

ahm

an e

t al

.(200

6)

El-R

ahm

an, K

. M. A

. , E

l-Kam

ash,

A. M

. , E

l-Sou

roug

y, M

. R. a

nd

Abd

el-M

onie

m, N

. M. :

The

rmod

ynam

ic m

odel

ing

for t

he re

mov

al

of C

s+, S

r2+ ,

Ca2

+ and

Mg2

+ ion

s fro

m a

queo

us w

aste

solu

tions

us

ing

zeol

ite A

, Jou

rnal

of R

adio

anal

ytic

al a

nd N

ucle

ar C

hem

istry

, vo

l.268

, No.

2, p

p.22

1-23

0 (2

006)

.

Ca,

Cs,

Mg,

Sr

zeol

ite

Ca,

Cs,

Mg,

Sr

solu

tion

13)

Ewar

t et a

l.(19

91)

Ewar

t, F.

, G

reen

field

, B

. F. ,

Haw

orth

, A

. , R

osev

ear,

A. a

nd

Will

iam

, S. J

. : T

he e

ffect

s of o

rgan

ics i

n SF

R o

n so

rptio

n co

effic

ient

s, SK

B P

RO

GR

ESS

REP

ORT

SFR

91-0

1 (1

991)

.

Pu

OPC

/BFS

, OPC

/BFS

/lim

esto

ne,

OPC

/BFS

/lim

esto

ne_i

ncl.S

P,

OPC

/PFA

, OPC

/PFA

_inc

l.SP,

SR

PC/li

mes

tone

, SR

PC/li

mes

tone

_inc

l.SP

leac

hing

OPC

:PFA

ce

men

t blo

cks,

leac

hing

Sol

id

- 12 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(3/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

14

) Fa

irhur

st e

t al.(

1995

) Fa

irhur

st, A

. J. ,

War

wic

k, P

. and

Ric

hard

son,

S. :

The

effe

ct o

f pH

on

eur

opiu

m-m

iner

al in

tera

ctio

ns in

the

pres

ence

of h

umic

aci

d,

Rad

ioch

imic

a Act

a, v

ol.6

9, p

p.10

3-11

1 (1

995)

.

Eu

bent

onite

, kao

lin,

mon

tmor

illon

ite, q

uartz

0.

05M

NaC

lO4

15)

Filip

ska

and

Stam

berg

(200

6)

Filip

ska,

H. a

nd S

tam

berg

, K. :

Sor

ptio

n of

Cs(

I) a

nd S

r(II

) on

a m

ixtu

re o

f ben

toni

te a

nd m

agne

tite

usin

g SC

M +

IExM

: A

para

met

ric st

udy,

Jour

nal o

f Rad

ioan

alyt

ical

and

Nuc

lear

C

hem

istry

, vol

.270

, No.

3, p

p.53

1-54

2 (2

006)

.

Cs,

Sr

bent

onite

, mag

netit

e 0.

001M

-0.5

M N

aNO

3

16)

Fras

ca e

t al.(

2014

) Fr

asca

, B. ,

Sav

oye,

S. ,

Witt

ebro

odt,

C. ,

Leu

pin,

O. X

. and

M

iche

lot,

J.-L.

: C

ompa

rativ

e st

udy

of S

e ox

yani

ons r

eten

tion

on

thre

e ar

gilla

ceou

s roc

ks: U

pper

Toa

rcia

n (T

ourn

emire

, Fra

nce)

, B

lack

Sha

les (

Tour

nem

ire, F

ranc

e) a

nd O

palin

us C

lay

(Mon

t Ter

ri,

Switz

erla

nd),

Jour

nal o

f Env

ironm

enta

l Rad

ioac

tivity

, vol

.127

, pp

.133

-140

(201

4).

Se

Bla

ck S

hale

s, O

PA, U

pper

To

arci

an

Pore

wat

er

17)

Gal

ambo

s et

al.(2

012)

G

alam

bos,

M. ,

Mag

ula,

M. ,

Dan

o, M

. , O

sack

y, M

. , R

ossk

opfo

va,

O. a

nd R

ajec

, P. :

Com

para

tive

stud

y of

ces

ium

ads

orpt

ion

on

dioc

tahe

dral

and

trio

ctah

edra

l sm

ectit

e, Jo

urna

l of R

adio

anal

ytic

al

and

Nuc

lear

Che

mis

try, v

ol.2

93, p

p.82

9-83

7 (2

012)

.

Cs

mon

tmor

illon

ite, s

apon

ite,

hect

orite

C

sCl

18)

Gao

et a

l.(20

15)

Gao

, Y. ,

Sha

o, Z

. and

Xia

o, Z

. : U

(VI)

sorp

tion

on il

lite:

effe

ct o

f pH

, ion

ic st

reng

th, h

umic

aci

d an

d te

mpe

ratu

re, J

ourn

al o

f R

adio

anal

ytic

al a

nd N

ucle

ar C

hem

istry

, vol

.303

, pp.

867-

876

(201

5).

U

illite

0.

001M

-0.1

M N

aNO

3

19)

Gha

yaza

et a

l.(20

11)

Gha

yaza

, M. ,

Le

Fore

stie

r, L.

, M

ulle

r, F.

, To

urna

ssat

, C. a

nd

Ben

y, J.

-M. :

Pb(

II) a

nd Z

n(II

) ads

orpt

ion

onto

Na-

and

C

a-m

ontm

orill

onite

in a

cetic

aci

d/ac

etat

e m

ediu

m: E

xper

imen

tal

appr

oach

and

geo

chem

ical

mod

elin

g, Jo

urna

l of C

ollo

id a

nd

Inte

rfac

e Sc

ienc

e, v

ol.3

61, p

p.23

8-24

6 (2

011)

.

Pb, Z

n C

a-, N

a-m

ontm

orill

onite

0.

02M

CaC

l 2, 0

.04M

N

aCl

20)

Gla

us a

nd V

an

Loon

(200

4)

Gla

us, M

. A. a

nd V

an L

oon,

L. R

. : A

gen

eric

pro

cedu

re fo

r the

as

sess

men

t of t

he e

ffect

of c

oncr

ete

adm

ixtu

res o

n th

e re

tent

ion

beha

viou

r of c

emen

t for

radi

onuc

lides

: Con

cept

and

cas

e st

udie

s, PS

I Ber

icht

04-

02, P

aul S

cher

rer I

nstit

ute

(200

4).

Eu, N

i, Th

ce

men

t pas

te_i

ncl.S

P A

rtific

ial c

emen

t por

e w

ater

- 13 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(4/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

21

) G

odel

itsas

et

al.(1

996)

G

odel

itsas

, A. ,

Mis

aelid

es, P

. , F

ilipp

idis

, A. ,

Cha

risto

s, D

. and

A

nous

is, I

. : U

rani

um so

rptio

n fr

om a

queo

us so

lutio

ns o

n so

dium

-for

m o

f HEU

-type

zeo

lite

crys

tals

, Jou

rnal

of

Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try, v

ol.2

08, N

o.2,

pp.

393-

402

(199

6).

U

Na-

zeol

ite

U so

lutio

n

22)

Gru

tter e

t al.(

1992

) G

rutte

r, A

. , v

on G

unte

n, H

. R. a

nd R

ossl

er, E

. : S

orpt

ion

of b

ariu

m

on u

ncon

solid

ated

gla

ciof

luvi

al d

epos

its a

nd c

lay

min

eral

s, R

adio

chim

ica A

cta,

vol

.58/

59, p

p.25

9-26

5 (1

992)

.

Ba

chlo

rite,

gla

ciof

luvi

al m

iner

als,

illite

, mon

tmor

illon

ite

synt

hetic

gro

undw

ater

23)

Gru

tter e

t al.(

1994

a)

Gru

tter,

A. ,

von

Gun

te, H

. R. ,

Ros

sler

, E. a

nd K

eil,

R. :

Sor

ptio

n of

N

icke

l and

Cob

alt o

n a

Size

-Fra

ctio

n of

Unc

onso

lidat

ed

Gla

ciof

luvi

al D

epos

its a

nd o

n C

lay

Min

eral

s, R

adio

chim

ica A

cta,

vo

l.65,

pp.

181-

187

(199

4).

Ba,

Co,

Cs,

Ni,

Sr

Gla

ciof

luvi

al m

iner

als,

mon

tmor

illon

ite, i

llite

, SiO

2 po

wde

r

synt

hetic

gro

undw

ater

24)

Gru

tter e

t al.(

1994

b)

Gru

tter,

A. ,

von

Gun

te, H

. R. ,

Ros

sler

, E. a

nd K

eil,

R. :

Sor

ptio

n of

St

ront

ium

on

Unc

onso

lidat

ed G

laci

oflu

vial

Dep

osits

and

on

Cla

y M

iner

als;

Mut

ual I

nter

fere

nce

of C

esiu

m, S

tront

ium

and

Bar

ium

, R

adio

chim

ica A

cta,

vol

.64,

pp.

247-

252

(199

4).

Ba,

Cs,

Sr

Gla

ciof

luvi

al m

iner

als,

chlo

rite,

ill

ite, m

ontm

orill

onite

sy

nthe

tic g

roun

dwat

er

25)

Gu

and

Evan

s(20

07)

Gu,

X. a

nd E

vans

, L. J

. : M

odel

ling

the

adso

rptio

n of

Cd(

II),

Cu(

II),

Ni(I

I), P

b(II

), an

d Zn

(II)

ont

o Fi

thia

n ill

ite, J

ourn

al o

f Col

loid

and

In

terf

ace

Scie

nce,

vol

.307

, pp.

317-

325

(200

7).

Cd,

Cu,

Ni,

Pb, Z

n ill

ite

0.00

1M-0

.1M

NaN

O3

26)

Guo

et a

l.(20

09)

Guo

, Z. ,

Xu,

J. ,

Shi,

K. ,

Tan

g, Y

. , W

u, W

. and

Tao

, Z. :

Eu(

III)

ad

sorp

tion/

deso

rptio

n on

Na-

bent

onite

: Exp

erim

enta

l and

mod

elin

g st

udie

s, C

ollo

ids a

nd S

urfa

ces A

: Phy

sico

chem

ical

and

Eng

inee

ring

Asp

ects

, vol

.339

, pp.

126-

133

(200

9).

Eu

Na-

bent

onite

0.

1M N

aCl

27)

Hou

et a

l.(20

15)

Hou

, Z. ,

Shi

, K. ,

Wan

g, X

. , Y

e, Y

. , G

uo, Z

. and

Wu,

W. :

In

vest

igat

ion

of S

e(IV

) sor

ptio

n on

Na-

kaol

inite

: bat

ch e

xper

imen

ts

and

mod

elin

g, Jo

urna

l of R

adio

anal

ytic

al a

nd N

ucle

ar C

hem

istry

, vo

l.303

, pp.

25-3

1 (2

015)

.

Se

Na-

kaol

inite

0.

001M

-0.1

M N

aCl

28)

Hsi

and

La

ngm

uir(

1985

) H

si, C

.-K. D

. and

Lan

gmui

r, D

. : A

dsor

ptio

n of

ura

nyl o

nto

ferr

ic

oxyh

ydro

xide

s: A

pplic

atio

n of

the

surf

ace

com

plex

atio

n si

te-b

indi

ng m

odel

, Geo

chim

ica

et C

osm

ochi

mic

a Act

a, v

ol.4

9,

pp.1

931-

1941

(198

5).

U

Fe(O

H) 3

(am

), go

ethi

te, h

emat

ite

0.1M

NaN

O3

- 14 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(5/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

29

) H

uitti

et a

l.(19

96)

Hui

tti, T

. , H

akan

en, M

. and

Lin

dber

g, A

. : S

orpt

ion

of c

esiu

m,

radi

um, p

rota

ctin

ium

, ura

nium

, nep

tuni

um a

nd p

luto

nium

on

rapa

kivi

gra

nite

, PO

SIVA

repo

rt, P

OSI

VA-9

6-23

(199

6).

Ba,

Cs,

Np,

Pa

, Pu,

U

gran

ite

Gro

undw

ater

30)

Iida

et a

l.(20

11)

Iida,

Y. ,

Tan

aka,

T. ,

Yam

aguc

hi, T

. and

Nak

ayam

a, S

. : S

orpt

ion

beha

vior

of s

elen

ium

(-II

) on

rock

s und

er re

duci

ng c

ondi

tions

, Jo

urna

l of N

ucle

ar S

cien

ce a

nd T

echn

olog

y, v

ol.4

8, N

o.2,

pp

.279

-291

(201

1).

Se

albi

te, b

iotit

e, c

alci

te, c

hlor

ite,

goet

hite

, gra

nodi

orite

, m

ontm

orill

onite

, pyr

ite, q

uartz

, sa

ndy

mud

ston

e, tu

fface

ous

sand

ston

e

0.05

M, 0

.5M

NaC

l, gr

ound

wat

er

31)

Iida

et a

l.(20

14)

Iida,

Y. ,

Yam

aguc

hi, T

. and

Tan

aka,

T. :

Sor

ptio

n be

havi

or

hydr

osel

enid

e (H

Se－

) ont

o iro

n-co

ntai

ning

min

eral

s, Jo

urna

l of

Nuc

lear

Sci

ence

and

Tec

hnol

ogy,

vol

.51,

No.

3, p

p.30

5-32

2 (2

014)

.

Se

biot

ite, f

erro

us o

xide

, goe

thite

, m

agne

tite

0.01

M-1

M N

aCl

32)

Jan

et a

l.(20

14)

Jan,

Y.-L

. , T

sai,

S.-S

. and

Li,

Y.-Y

. : D

eter

min

atio

n of

sorp

tion

and

diffu

sion

par

amet

ers o

f Se(

IV) o

n cr

ushe

d gr

anite

, Jou

rnal

of

Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try, v

ol.3

01, p

p.36

5-37

1 (2

014)

.

Se

gran

ite

GW

, SW

33)

Jin

et a

l.(20

14)

Jin,

Q. ,

Wan

g, G

. , G

e, M

. , C

hen,

Z. ,

Wu,

W. a

nd G

uo, Z

. : T

he

adso

rptio

n of

Eu(

III)

and

Am

(III

) on

Bei

shan

gra

nite

: XPS

, EPM

A,

batc

h an

d m

odel

ing

stud

y, A

pplie

d G

eoch

emis

try, v

ol.4

7, p

p.17

-24

(201

4).

Am

, Eu

gran

ite

0.03

3M C

aCl 2,

0.1

M

NaC

l, sy

nthe

tic

grou

ndw

ater

34)

Kas

ar e

t al.(

2014

) K

asar

, S. ,

Kum

ar, S

. , K

ar, A

. , B

ajpa

i, R

. K. ,

Kau

shik

, C. P

. and

To

mar

, B. S

. : R

eten

tion

beha

viou

r of C

s(I)

, Sr(

II),

Tc(V

II) a

nd

Np(

V) o

n sm

ectit

e-ric

h cl

ay, J

ourn

al o

f Rad

ioan

alyt

ical

and

Nuc

lear

C

hem

istry

, vol

.300

, pp.

71-7

5 (2

014)

.

Cs,

Np,

Sr,

Tc

clay

0.

01M

-1M

NaC

l

35)

Koh

ler e

t al.(

1999

) K

ohle

r, M

. , H

oney

man

, B. D

. and

Lec

kie,

J. O

. : N

eptu

nium

(V)

sorp

tion

on h

emat

ite (

-Fe 2

O3)

in a

queo

us su

spen

sion

: The

effe

ct o

f C

O2,

Rad

ioch

imic

a A

cta,

vol

.85,

pp.

33-4

8 (1

999)

.

Np

goet

hite

, hem

atite

, qua

rtz

0.00

5M-0

.1M

N

aClO

4

36)

Koh

licko

va a

nd

Jedi

nako

va-

Kriz

ove(

1998

)

Koh

licko

va, M

. and

Jedi

nako

va-K

rizov

e, V

. : E

ffect

of p

H a

nd E

h on

the

sorp

tion

of se

lect

ed ra

dion

uclid

es, J

ourn

al o

f Rad

ioan

alyt

ical

an

d N

ucle

ar C

hem

istry

, vol

.229

, No.

1-2,

pp.

43-4

8 (1

998)

.

Cs,

I, Sr

, Tc

be

nton

ite

synt

hetic

gro

undw

ater

- 15 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(6/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

37

) K

ulm

ala

and

Hak

anen

(199

5)

Kul

mal

a, S

. and

Hak

anen

, M. :

Sor

ptio

n of

alk

alin

e-ea

rth e

lem

ents

Sr

, Ba

and

Ra

from

gro

undw

ater

on

rock

s fro

m T

VO

inve

stig

atio

n ar

eas,

Nuc

lear

Was

te C

omm

issi

on o

f Fin

nish

Pow

er C

ompa

nies

, Y

JT-9

5-03

(199

5).

Ba,

Ra,

Sr

gran

ite, m

ica

gnei

ss, t

onal

ite

fres

h gr

ound

wat

er,

salin

e gr

ound

wat

er

38)

Kul

mal

a et

al.(

1996

) K

ulm

ala,

S. ,

Hak

anen

, M. a

nd L

indb

erg,

A. :

Sor

ptio

n of

pr

otac

tiniu

m o

n ro

cks i

n gr

ound

wat

ers f

rom

Pos

iva

inve

stig

atio

n si

tes,

POSI

VA-9

6-18

(199

6)

Pa

gran

ite, m

ica

gnei

ss, t

onal

ite

Gro

undw

ater

39)

Kum

ar e

t al.(

2013

) K

umar

, S. ,

Pen

te, A

. S. ,

Baj

pai,

R. K

. , K

aush

ik, C

. P. a

nd T

omar

, B

. S. :

Am

eric

ium

sorp

tion

on s

mec

tite-

rich

natu

ral c

lay

from

gr

aniti

c gr

ound

wat

er, A

pplie

d G

eoch

emis

try, v

ol.3

5, p

p.28

-34

(201

3).

Am

, Eu

Na-

clay

, Ca-

clay

, nat

ural

cla

y,

mon

tmor

illon

ite

0.01

M-0

.1M

NaC

l, 0.

0335

M C

aCl 2,

0.

035M

Na 2

SO4,

0.1M

NaN

O3,

grou

ndw

ater

40

) K

unim

aru

et a

l.(20

12)

Kun

imar

u, T

. , M

orik

awa,

K. ,

Tac

hi, Y

. , K

uno,

Y. ,

Hos

oya,

S. ,

Sh

imod

a, S

. , K

ato,

H. ,

Nak

azaw

a, T

. , Ik

use,

H. a

nd K

ubot

a, M

. :

Mea

sure

men

ts o

f Sor

ptio

n, D

iffus

ion

and

Pore

Phy

sica

lity

for

Gra

nite

Sam

ple,

JAEA

Tec

hnic

al R

epor

t, JA

EA-D

ata/

Cod

e 20

12-0

13 (2

012)

, 96p

.

Cs,

Sr

gran

ite-f

ract

ure,

gra

nite

-Int

act

0.5M

NaC

l, gr

ound

wat

er

41)

Kyl

lone

n et

al.(

2008

) K

yllo

nen,

J. ,

Hak

anen

, M. a

nd L

indb

erg,

A. :

Sor

ptio

n of

Ces

ium

on

Olk

iluot

o M

ica

Gne

iss a

nd G

rano

dior

ite in

Sal

ine

Gro

undw

ater

; R

etar

datio

n of

Ces

ium

Tra

nspo

rt in

Roc

k Fr

actu

re C

olum

ns,

POSI

VA, W

orki

ng R

epor

t 200

8-62

(200

8).

Cs

biot

ite

0.1M

CaC

l 2, 0

.1M

K

Cl,

0.1M

NaC

l

42)

Lee

et a

l.(20

06)

Lee,

C.-P

. , L

an, P

.-L. ,

Jan,

Y.-L

. , W

ei, Y

.-Y. ,

Ten

g, S

.-P. a

nd H

su,

C.-N

. : S

orpt

ion

of c

esiu

m o

n gr

anite

und

er a

erob

ic a

nd a

naer

obic

co

nditi

ons,

Rad

ioch

imic

a Act

a, v

ol.9

4, p

p.67

9-68

2 (2

006)

.

Cs

gran

ite

SGW

43)

Lee

et a

l.(20

07)

Lee,

C.-P

. , Ja

n, Y

.-L. ,

Lan

, P.-L

. , W

ei, Y

.-Y. ,

Ten

g, S

.-P. a

nd H

su,

C.-N

. : A

naer

obic

and

aer

obic

sorp

tion

of c

esiu

m a

nd se

leni

um o

n m

udro

ck, J

ourn

al o

f Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try,

vol.2

74, N

o.1,

pp.

145-

151

(200

7).

Cs,

Se

mud

ston

e SG

W

44)

Lee

et a

l.(20

12)

Lee,

C.-P

. , W

u, M

.-C. ,

Tsa

i, T.

-L. ,

Wei

, H.-J

. , M

en, L

.-C. a

nd L

in,

T.-Y

. : C

ompa

rativ

e st

udy

on re

tard

atio

n be

havi

or o

f Cs i

n cr

ushe

d an

d in

tact

rock

s: tw

o po

tent

ial r

epos

itory

hos

t roc

ks in

the

Taiw

an

area

, Jou

rnal

of R

adio

anal

ytic

al a

nd N

ucle

ar C

hem

istry

, vol

.293

, pp

.579

-586

(201

2).

Cs

basa

lt, g

rani

te

de-io

nize

d w

ater

- 16 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(7/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

45

) Le

e et

al.(

2013

a)

Lee,

C.-P

. , L

iu, C

.-Y. ,

Wu,

M.-C

. , P

an, C

.-H. ,

Tsa

i, T.

-L. ,

Wei

, H

.-J. a

nd M

en, L

.-C. :

Sim

ulat

ion

of a

2-s

ite L

angm

uir m

odel

for

char

acte

rizin

g th

e so

rptio

n ca

paci

ty o

f Cs a

nd S

e in

cru

shed

m

udro

ck u

nder

var

ious

ioni

c st

reng

th e

ffect

s, Jo

urna

l of

Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try, v

ol.2

96, p

p.11

19-1

125

(201

3).

Cs,

Se

mud

ston

e gr

ound

wat

er,

seaw

ater

46)

Lee

et a

l.(20

13b)

Le

e, C

.-P. ,

Liu

, C.-Y

. , W

u, M

.-C. ,

Pan

, C.-H

. , T

sai,

T.-L

. , L

in,

T.-Y

. , W

ei, H

.-J. a

nd M

en, L

.-C. :

App

licat

ion

of n

on-li

near

he

tero

gene

ity-b

ased

isot

herm

mod

els f

or c

hara

cter

izin

g so

rptio

n of

C

s and

Se

on m

udro

cks,

Jour

nal o

f Rad

ioan

alyt

ical

and

Nuc

lear

C

hem

istry

, vol

.298

, pp.

749-

754

(201

3).

Cs,

Se

mud

ston

e Se

awat

er

47)

Lee(

1973

) Le

e, S

. H. :

Stu

dies

on

the

Sorp

tion

and

Fixa

tion

of C

esiu

m b

y Ve

rmic

ulite

, Jou

rnal

of t

he K

orea

n N

ucle

ar S

ocie

ty, v

ol.5

, No.

4,

pp.3

10-3

20 (1

973)

.

Cs

K-v

erm

icul

ite,

Nat

ural

-ver

mic

ulite

, N

a-ve

rmic

ulite

0.3M

NaN

O3

48)

Luja

nien

e et

al.(

2010

) Lu

jani

ene,

G. ,

Ben

es, P

. , S

tam

berg

, K. ,

Sap

olai

te, J

. , V

opal

ka,

D. ,

Rad

ziut

e, E

. and

Sei

glo,

T. :

Effe

ct o

f nat

ural

cla

y co

mpo

nent

s on

sorp

tion

of C

s, Pu

and

Am

by

the

clay

, Jou

rnal

of

Rad

ioan

alyt

ical

and

Nuc

lear

Che

mis

try, v

ol.2

86, p

p.35

3-35

9 (2

010)

.

Am

, Cs,

Pu

clay

, goe

thite

, hem

atite

, mag

netit

e 0.

01M

, 0.1

M N

aNO

3

49)

Mae

s and

C

rem

ers(

1986

) M

aes,

A. a

nd C

rem

ers,

A. :

Eur

opiu

m so

rptio

n on

a c

lay

sedi

men

t: Su

lpha

te a

nd io

nic

stre

ngth

effe

cts,

Envi

ronm

enta

l Sci

ence

s, pp

.103

-110

(198

6).

Eu

Mg-

clay

, Mg-

mon

tmor

illon

ite,

Na-

clay

, Na-

mon

tmor

illon

ite

0.1N

-0.4

M

Mg(

NO

3)2+

MgS

O4,

0.1N

-0.4

N

NaN

O3+

Na 2

SO4

50)

Mar

ques

Fer

nand

es e

t al

.(201

2)

Mar

ques

Fer

nand

es, M

. , B

aeye

ns, B

. , D

ahn,

R. ,

Sch

eino

st, A

. C.

and

Bra

dbur

y, M

. H. :

U(V

I) so

rptio

n on

mon

tmor

illon

ite in

the

abse

nce

and

pres

ence

of c

arbo

nate

: A m

acro

scop

ic a

nd m

icro

scop

ic

stud

y, G

eoch

imic

a et

Cos

moc

him

ica A

cta,

vol

.93,

pp.

262-

277

(201

2).

U

Swy-

1 m

ontm

orill

onite

0.

1M N

aClO

4

51)

Mar

ques

Fer

nand

es e

t al

.(201

5)

Mar

ques

Fer

nand

es, M

. , V

er, N

. and

Bae

yens

, B. :

Pre

dict

ing

the

upta

ke o

f Cs,

Co,

Ni,

Eu, T

h an

d U

on

argi

llace

ous r

ocks

usi

ng

sorp

tion

mod

els f

or il

lite,

App

lied

Geo

chem

istry

, vol

.59,

pp

.189

-199

(201

5).

Co,

Cs,

Eu,

Ni,

Th, U

cl

ay, i

llite

0.

1M N

aClO

4, sy

nthe

tic p

orew

ater

- 17 -


Tabl

e 3.

1 O

verv

iew

of 8

3 re

fere

nces

sel

ecte

d fo

r upd

atin

g th

e JA

EA-S

DB

(8/1

1)

No.

R

efer

ence

D

etai

ls o

f ref

eren

ce

Elem

ent

Solid

Pha

se

Solu

tion

Type

52

) M

issa

na e

t al.(

2013

) M

issa

na, T

. , B

ened

icto

, A. ,

Gar

cia-

Gut

ierr

ez, M

. and

Alo

nso,

U. :

M

odel

ing

cesi

um re

tent

ion

onto

Na-

, K- a

nd C

a-sm

ectit

e: E

ffect

s of

ioni

c st

reng

th, e

xcha

nge

and

com

petin

g ca

tions

on

the

dete

rmin

atio

n of

sele

ctiv

ity c

oeffi

cien

ts, G

eoch

imic

a et

C

osm

ochi

mic

a Act

a, v

ol.1

28, p

p.26

6-27

7 (2

014)

.

Cs

Ca-

, K-,

Na-

smec

tite

0.00

1M-1

M N

aClO

4, 0.

03M

-0.1

M C

aCl 2,

0.

01M

-0.1

M K

Cl

53)

Mis

sana

et a

l.(20

14)

Mis

sana

, T. ,

Gar

cia-

Gut

ierr

ez, M

. , B

ened

icto

, A. ,

Ayo

ra, C

. and

D

e-Po

urcq

, K. :

Mod

elin

g of

Cs a

dsor

ptio

n in

nat

ural

mix

ed-c

lay

and

the

effe

cts o

f ion

com

petit

ion,

App

lied

Geo

chem

istry

, vol

.49,

pp

.95-

102

(201

4).

Cs

Ca-

, K-,

Na-

, NH

4-ill

ite, C

a-, K

-, N

a-, N

H4-

kaol

inite

, RC

cla

y, S

J cl

ay

0.1M

CaC

l 2, 0

.1M

K

Cl,

0.1M

NH

4Cl,

0.1M

, 0.5

M N

aCl,

natu

ral s

alin

e w

ater

54

) M

uurin

en a

nd

Tour

nass

at(2

011)

M

uurin

en, A

. and

Tou

rnas

sat,

C. :

Sor

ptio

n an

d D

iffus

ion

of F

e(II

) in

Ben

toni

te -S

orpt

ion

Stud

ies-

, PO

SIVA

, Wor

king

Rep

ort 2

011-

09

(201

1).

Fe

MX

-80,

smec

tite

0.05

M, 0

.3M

NaC

l

55)

Muu

rinen

et a

l.(20

14)

Muu

rinen

, A. ,

Tou

rnas

sat,

C. ,

Had

i, J.

, Gre

nech

e, J.

-M. :

Sor

ptio

n an

d di

ffusi

on o

f Fe(

II) i

n be

nton

ite, W

orki

ng R

epor

ts c

onta

in

info

rmat

ion

on w

ork

in p

rogr

ess o

r pen

ding

com

plet

ion,

Wor

king

R

epor

t 201

4-04

(201

4).

Fe

MX

-80,

smec

tite

0.05

M, 0

.3M

NaC

l

56)

Nak

ata

et a

l.(20

00)

Nak

ata,

K. ,

Nag

asak

i, S.

, Ta

naka

, S. ,

Sak

amot

o, Y

. , T

anak

a, T

. an

d O

gaw

a, H

. : S

orpt

ion

and

redu

ctio

n of

nep

tuni

um(V

) on

the

surf

ace

of ir

on o

xide

s, R

adio

chim

ica A

cta,

vol

.90,

pp.

665-

669

(200

2).

Np

mag

netit

e, h

emat

ite

0.1M

NaN

O3

57)

Nak

ata

et a

l.(20

02)

Nak

ata,

K. ,

Nag

asak

i, S.

, Ta

naka

, S. ,

Sak

amot

o, Y

. , T

anak

a, T

. an

d O

gaw

a, H

. : S

orpt

ion

and

deso

rptio

n ki

netic

s of N

p(V

) on

mag

netit

e an

d he

mat

ite, R

adio

chim

ica A

cta,

vol

.88,

pp.

453-

457

(200

0).

Np

mag

netit

e, h

emat

ite

0.1M

NaN

O3

58)

Neb

elun

g an

d B

rend

ler(

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