Radionuclide and Metal Sorption on Cement and Concrete (eBook)

Michael Ochs, Dirk Mallants, Lian Wang (Autoren)

eBook Download: PDF

2015 | 1st ed. 2016
XXX, 301 Seiten
Springer International Publishing (Verlag)
978-3-319-23651-3 (ISBN)

Infos

Cementitious materials are being widely used as solidification/stabilisation and barrier materials for a variety of chemical and radioactive wastes, primarily due to their favourable retention properties for metals, radionuclides and other contaminants. The retention properties result from various mineral phases in hydrated cement that possess a high density and diversity of reactive sites for the fixation of contaminants through a variety of sorption and incorporation reactions.

This book presents a state of the art review and critical evaluation of the type and magnitude of the various sorption and incorporation processes in hydrated cement systems for twenty-five elements relevant for a broad range of radioactive and industrial wastes. Effects of cement evolution or ageing on sorption/incorporation processes are explicitly evaluated and quantified. While the immobilisation of contaminants by mixing-in during hydration is not explicitly addressed, the underlying chemical processes are similar.

A quantitative database on the solid/liquid distribution behaviour of radionuclides and other elements in hydrated cement systems is established on the basis of a consistent review and re-evaluation of literature data. In addition to recommended values, all underlying original experimental data and key experimental info

rmation are provided, which allows users to trace the given recommendations or to develop their own set of key values.

This database is closely tied to the safety analysis of near surface disposal of radioactive waste in Belgium. It focuses on radioelements, toxic stable elements and heavy metals, which makes it relevant for investigations involving the interaction of radioactive and conventional contaminants with cement-based barriers.

Inhalt

Preface 6
Contents 7
Acronyms 12
Symbols 14
List of Figures 16
List of Tables 27
1 Introduction and Objective 29
Abstract 29
References 31
2 Cementitious Materials and Their Sorption Properties 32
Abstract 32
2.1 Cementitious Materials 32
2.2 Cement 33
2.3 Cement Hydration 34
2.4 Sorbing Minerals in Cementitious Materials 34
2.5 Degradation of Hydrated Cement 38
2.5.1 Degradation States 38
2.5.2 Illustrative Example 40
References 42
3 Sorption Values for Chlorine and Iodine 44
Abstract 44
3.1 Chlorine 44
3.1.1 Chemical Form, Speciation, and Solubility 44
3.1.2 Sorption Values from the Literature for the Benchmark Cement 47
3.1.3 Sorption Mechanisms and Selected Sorption Values 50
3.1.3.1 Influence of Chloride Concentration on Chloride Sorption Values 50
3.1.3.2 Grouping of Rd Values as a Function of Total Aqueous Chloride Concentration 51
3.1.3.3 Influence of pH on Chloride Sorption Values 54
3.1.3.4 Rd Values at a Low Aqueous Cl Concentration 55
3.1.3.5 Rd Values at a High Aqueous Cl Concentration 56
3.1.3.6 Sorption Mechanisms 56
3.1.3.7 Sorption at State I 59
3.1.3.8 Sorption at State II 59
3.1.3.9 Sorption at State III 59
3.1.3.10 Sorption at State IV 60
3.2 Iodine 60
3.2.1 Chemical Form, Speciation, and Solubility 60
3.2.2 Sorption Values from the Literature for the Benchmark Cement 62
3.2.3 Sorption Mechanisms and Selected Sorption Values 64
3.2.3.1 Influence of pH on Iodine Sorption 64
3.2.3.2 Influence of Aqueous Concentration of Chlorine 65
3.2.3.3 Sorption Mechanisms 66
3.2.3.4 Sorption at State I 67
3.2.3.5 Sorption at State II 68
3.2.3.6 Sorption at State III 68
3.2.3.7 Sorption at State IV 68
References 68
4 Sorption Values for Caesium, Strontium, Radium, and Silver 72
Abstract 72
4.1 Caesium 72
4.1.1 Chemical Form, Speciation, and Solubility 72
4.1.2 Sorption Values from the Literature for the Benchmark Cement 73
4.1.2.1 Cement Pastes Rd Values 75
4.1.2.2 CSH Phases Rd Values 76
4.1.3 Sorption Mechanisms and Selected Sorption Values 77
4.1.3.1 Sorption Mechanisms 77
4.1.3.2 Sorption at State I 81
4.1.3.3 Sorption at State II 82
4.1.3.4 Sorption at State III 82
4.1.3.5 Sorption at State IV 83
4.2 Strontium 83
4.2.1 Chemical Form, Speciation, and Solubility 83
4.2.2 Sorption Values from the Literature for the Benchmark Cement 85
4.2.3 Sorption Mechanisms and Selected Sorption Values 87
4.2.3.1 Sorption Mechanisms 87
4.2.3.2 Sorption at State I 90
4.2.3.3 Sorption at State II 90
4.2.3.4 Sorption at State III 90
4.2.3.5 Sorption at State IV 90
4.3 Radium 91
4.3.1 Chemical Form, Speciation, and Solubility 91
4.3.2 Sorption Values from the Literature for the Benchmark Cement 92
4.3.3 Sorption Mechanisms and Selected Sorption Values 94
4.3.3.1 Sorption Mechanisms 94
4.3.3.2 Sorption at State I 96
4.3.3.3 Sorption at State II 96
4.3.3.4 Sorption at State III 96
4.3.3.5 Sorption at State IV 97
4.4 Silver 97
4.4.1 Chemical Form, Speciation and Solubility 97
4.4.2 Sorption Values from the Literature for the Benchmark Cement 101
4.4.3 Sorption Mechanisms and Selected Sorption Values 102
4.4.4 Supplemental Values for Safety Assessment Calculations 103
References 103
5 Sorption Values for Calcium, Nickel, and Carbon 107
Abstract 107
5.1 Calcium 107
5.1.1 Chemical Form, Speciation, and Solubility 107
5.1.2 Literature Information, Mechanisms, and Selected Sorption Values 109
5.2 Nickel 113
5.2.1 Chemical Form, Speciation, and Solubility 113
5.2.2 Sorption Values from the Literature for the Benchmark Cement 116
5.2.3 Sorption Mechanisms and Selected Sorption Values 124
5.2.3.1 Sorption Mechanisms 124
5.2.3.2 Approach to Derive Sorption Values Taking Account of Stable Nickel 125
5.2.3.3 Sorption at State I 128
5.2.3.4 Sorption at State II 128
5.2.3.5 Sorption at State III 129
5.2.3.6 Sorption at State IV 129
5.3 Carbon 129
5.3.1 Chemical Form, Speciation, and Solubility 129
5.3.2 Sorption Values from the Literature for the Benchmark Cement 132
5.3.2.1 Introduction 132
5.3.2.2 Sorption Values 134
Concrete Rd Values 136
Cement Paste Rd Values 137
CSH-Phase Kd-Values 138
Calcite-Phase Kd-Values 139
5.3.2.3 14C Partitioning Between Organic and Inorganic Carbons 139
5.3.3 Sorption Mechanisms and Selected Sorption Values 140
5.3.3.1 Factors Influencing Rd on the Benchmark Cement 140
5.3.3.2 Sorption Mechanisms 141
5.3.3.3 Sorption at State I 142
5.3.3.4 Sorption at State II 142
5.3.3.5 Sorption at State III 142
5.3.3.6 Sorption at State IV 142
References 143
6 Sorption Values for Thorium, Uranium, Plutonium, Neptunium, and Protactinium 147
Abstract 147
6.1 Thorium 147
6.1.1 Chemical Form, Speciation, and Solubility 147
6.1.2 Sorption Values from the Literature for the Benchmark Cement 150
6.1.3 Sorption Mechanisms and Selected Sorption Values 153
6.1.3.1 Influence of SL Ratio 153
6.1.3.2 Influence of Cement Degradation 157
6.1.3.3 Impacts of High Chlorine Concentration on Sorption 157
6.1.3.4 Sorption Mechanisms 157
6.1.3.5 Sorption at State I 159
6.1.3.6 Sorption at State II 159
6.1.3.7 Sorption at State III 159
6.1.3.8 Sorption at State IV 160
6.2 Uranium 160
6.2.1 Chemical Form, Speciation, and Solubility 160
6.2.2 Sorption Values from the Literature for the Benchmark Cement 163
6.2.3 Sorption Mechanisms and Selected Sorption Values 166
6.2.3.1 Sorption Mechanisms 166
6.2.3.2 Sorption at State I 168
6.2.3.3 Sorption at State II 168
6.2.3.4 Sorption at State III 169
6.2.3.5 Sorption at State IV 169
6.3 Plutonium 170
6.3.1 Chemical Form, Speciation, and Solubility 170
6.3.2 Sorption Values from the Literature for the Benchmark Cement 174
6.3.3 Sorption Mechanisms and Selected Sorption Values 178
6.3.3.1 Sorption Mechanisms 178
6.3.3.2 Sorption in State I 180
6.3.3.3 Sorption in State II 180
6.3.3.4 Sorption in State III 180
6.3.3.5 Sorption in State IV 181
6.4 Neptunium 181
6.4.1 Chemical Form, Speciation, and Solubility 181
6.4.2 Sorption Values from the Literature for the Benchmark Cement 185
6.4.3 Sorption Mechanisms and Selected Sorption Values 187
6.4.3.1 Sorption Mechanisms 187
6.4.3.2 Sorption at State I 188
6.4.3.3 Sorption at State II 188
6.4.3.4 Sorption at State III 188
6.4.3.5 Sorption at State IV 189
6.4.3.6 Sorption Values for Np(V) 189
6.5 Protactinium 189
6.5.1 Chemical Form, Speciation, and Solubility 189
6.5.2 Sorption Values from the Literature for the Benchmark Cement 190
6.5.3 Sorption Mechanisms and Selected Sorption Values 192
6.5.3.1 Sorption Mechanisms 192
6.5.3.2 Sorption at States I, II, III, and IV 192
References 193
7 Sorption Values for Americium 197
Abstract 197
7.1 Chemical Form, Speciation, and Solubility 197
7.2 Sorption Values from the Literature for the Benchmark Cement 198
7.2.1 Reviewed Sorption Values for Am and Eu 199
7.2.2 Europium as a Chemical Analogue for Americium in Sorption Experiments 202
7.3 Sorption Mechanisms and Selected Sorption Values 203
7.3.1 Sorption Mechanisms 203
7.3.1.1 Solid-to-Liquid Ratio 204
7.3.1.2 Cement Degradation 205
7.3.1.3 Sorption Reversibility 205
7.3.2 Sorption at State I 205
7.3.3 Sorption at State II 206
7.3.4 Sorption at State III 206
7.3.5 Sorption at State IV 206
References 207
8 Sorption Values for Selenium, Molybdenum, and Technetium 209
Abstract 209
8.1 Selenium 209
8.1.1 Chemical Form, Speciation, and Solubility 209
8.1.2 Sorption Values from the Literature for the Benchmark Cement 215
8.1.3 Sorption Mechanisms and Selected Sorption Values 217
8.1.3.1 Sorption Mechanisms 217
8.1.3.2 Sorption at State I 219
8.1.3.3 Sorption at State II 219
8.1.3.4 Sorption at State III 220
8.1.3.5 Sorption at State IV 220
8.1.4 Supplemental Values for Assessment Calculations 221
8.2 Molybdenum 221
8.2.1 Chemical Form, Speciation, and Solubility 221
8.2.2 Sorption Values from the Literature for the Benchmark Cement 224
8.2.3 Sorption Mechanisms and Selected Sorption Values 224
8.3 Technetium 225
8.3.1 Chemical Form, Speciation, and Solubility 225
8.3.2 Sorption Values from the Literature for the Benchmark Cement 229
8.3.3 Sorption Mechanisms and Selected Sorption Values 231
8.3.3.1 Sorption Mechanisms 231
Tc(VII) 232
Tc(IV) 232
8.3.3.2 Sorption at State I 232
8.3.3.3 Sorption at State II 233
8.3.3.4 Sorption at State III 233
8.3.3.5 Sorption at State IV 233
References 233
9 Sorption Values for Palladium and Lead 236
Abstract 236
9.1 Palladium 236
9.1.1 Chemical Form, Speciation, and Solubility 236
9.1.2 Literature Information, Mechanisms, and Selected Sorption Values 238
9.1.3 Supplemental Values for Assessment Calculations 239
9.2 Lead 240
9.2.1 Chemical Form, Speciation, and Solubility 240
9.2.2 Sorption Values from the Literature for the Benchmark Cement 240
9.2.3 Sorption Mechanisms and Selected Sorption Values 241
9.2.3.1 Lead Sorption at State I 242
9.2.3.2 Lead Sorption at State II 243
9.2.3.3 Lead Sorption at State III 243
9.2.3.4 Lead Sorption at State IV 243
References 244
10 Sorption Values for Niobium and Tin 245
Abstract 245
10.1 Niobium 245
10.1.1 Chemical Form, Speciation and Solubility 245
10.1.2 Sorption Values from the Literature for the Benchmark Cement 248
10.1.3 Sorption Mechanisms and Selected Sorption Values 248
10.1.3.1 Sorption Mechanisms 249
10.1.3.2 Sorption at State I 250
10.1.3.3 Sorption at State II 250
Sorption at State III 250
10.1.3.4 Sorption at State IV 250
10.2 Tin 251
10.2.1 Chemical Form, Speciation, and Solubility 251
10.2.2 Sorption Values from the Literature for the Benchmark Cement 255
10.2.3 Sorption Mechanisms and Selected Sorption Values 256
10.2.3.1 Sorption Mechanisms 256
10.2.3.2 Sorption at State I 256
10.2.3.3 Sorption at State II 257
10.2.3.4 Sorption at State III 258
10.2.3.5 Sorption at State IV 258
10.2.4 Supplemental Values for Assessment Calculations 258
10.2.4.1 Supplemental Values for State III 258
10.2.4.2 Supplemental Values for State IV 259
References 259
11 Sorption Values for Hydrogen and Beryllium 261
Abstract 261
11.1 Hydrogen (Tritium) 261
11.1.1 Chemical Form, Speciation, and Solubility 261
11.1.2 Sorption Values from the Literature for the Benchmark Cement 262
11.1.3 Sorption Mechanisms and Selected Sorption Values 262
11.1.3.1 Sorption Mechanisms 263
11.1.3.2 Sorption at States I, II, III, and IV 263
11.2 Beryllium 263
11.2.1 Chemical Form, Speciation, and Solubility 263
11.2.2 Sorption Values from the Literature for the Benchmark Cement 264
11.2.3 Sorption Mechanisms, Selected Sorption Values, and Supplemental Values 264
References 265
12 Sorption Values for Zirconium 266
Abstract 266
12.1 Chemical Form, Speciation, and Solubility 266
12.2 Sorption Values from the Literature for the Benchmark Cement 269
12.3 Sorption Mechanisms and Selected Sorption Values 270
12.3.1 Sorption Mechanisms 271
12.3.2 Sorption at State I 271
12.3.3 Sorption at State II 272
12.3.4 Sorption at State III 272
12.3.5 Sorption at State IV 273
12.4 Supplemental Values for Safety Assessment Calculations 273
12.4.1 Supplemental Values for State I 273
12.4.2 Supplemental Values for State IV 273
References 274
Annex Summary Tables with Sorption Data 275
Bibliography 316

Produkt-Details

• Erscheint lt. Verlag: 17.10.2015
• Reihe/Serie: Topics in Safety, Risk, Reliability and Quality
• Reihe/Serie: Topics in Safety, Risk, Reliability and Quality
• Zusatzinfo: XXX, 301 p.
• Verlagsort: Cham
• Sprache: englisch
• Themenwelt: Naturwissenschaften ► Physik / Astronomie
• Themenwelt: Technik ► Bauwesen
• Themenwelt: Technik ► Maschinenbau
• Schlagworte: Cement and Concrete • Geochemistry • radionuclides and metals • Sorption • thermodynamics • waste management
• ISBN-10: 3-319-23651-2 / 3319236512
• ISBN-13: 978-3-319-23651-3 / 9783319236513