Eh-pH Diagrams by Sushanta K Sahu

Atlas of Eh-pH diagrams Intercomparison of thermodynamic databases Geological Survey of Japan Open File Report No.419

National Institute of Advanced Industrial Science and Technology Research Center for Deep Geological Environments Naoto TAKENO May 2005

Contents 1 Introduction

2 Databases

3 Method for constructing Eh-pH diagrams 3.1 FACT/FACTSAGE . . . . . . . . . . . . 3.2 SUPCRT/FLASK-AQ . . . . . . . . . . . 3.3 LLNL/GWB . . . . . . . . . . . . . . . . 3.4 JNC-TDB/GWB . . . . . . . . . . . . . . 3.5 HATCHES/FLASK-AQ . . . . . . . . . . 3.6 OECD/NEA . . . . . . . . . . . . . . . . 3.7 OECD-NEA update . . . . . . . . . . . .

. . . . . . .

8 9 9 9 9 9 9 10

4 Explanation of the diagrams and tables

5 Reliability and uncertainty

6 Description of the softwares and their execution environments

List of Tables 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51

List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List

of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of

softwares used Ac species . . . Ag species . . . Al species . . . Am species . . As species . . . Au species . . . B species . . . Ba species . . . Be species . . . Bi species . . . Br species . . . C species (1) . C species (2) . Ca species . . . Cd species . . . Ce species . . . Cl species . . . Cm species . . Co species . . . Cr species . . . Cs species . . . Cu species . . . Dy species . . . Er species . . . Eu species . . . F species . . . Fe species . . . Fr species . . . Ga species . . . Gd species . . . Ge species . . . Hf species . . . Hg species . . . Ho species . . . I species . . . . In species . . . K species . . . La species . . . Li species . . . Lu species . . . Mg species . . Mn species . . Mo species . . N species . . . Na species . . . Nb species . . . Nd species . . . Ni species . . . Np species . . . Os species . . .

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

11 13 17 21 25 29 32 35 39 43 46 48 50 51 55 59 63 66 69 73 77 81 85 88 90 93 97 101 104 106 108 110 112 115 118 121 124 127 131 135 138 141 145 149 153 157 161 165 169 173 176

52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86

List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List List

of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of

P species . Pa species . Pb species . Pd species . Pm species Po species . Pr species . Pt species . Pu species . Ra species . Rb species . Re species . Rh species . Ru species . S species . . Sb species . Sc species . Se species . Si species . Sm species . Sn species . Sr species . Tb species . Tc species . Te species . Th species . Tl species . Tm species U species . V species . W species . Y species . Yb species . Zn species . Zr species .

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

179 183 187 190 192 194 196 198 201 205 208 210 212 215 219 223 226 229 233 237 241 245 248 251 254 257 260 262 265 269 272 274 276 279 283

List of Figures 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51

Flow chart of creating this report . . . . . . Legend of Eh-pH diagram . . . . . . . . . . Eh-pH diagrams of the system Ac-O-H (1) . Eh-pH diagrams of the system Ac-O-H (2) . Eh-pH diagrams of the system Ag-O-H (1) . Eh-pH diagrams of the system Ag-O-H (2) . Eh-pH diagrams of the system Al-O-H (1) . Eh-pH diagrams of the system Al-O-H (2) . Eh-pH diagrams of the system Am-O-H (1) Eh-pH diagrams of the system Am-O-H (2) Eh-pH diagrams of the system As-O-H (1) . Eh-pH diagrams of the system As-O-H (2) . Eh-pH diagrams of the system Au-O-H . . . Eh-pH diagrams of the system B-O-H (1) . Eh-pH diagrams of the system B-O-H (2) . Eh-pH diagrams of the system Ba-O-H (1) . Eh-pH diagrams of the system Ba-O-H (2) . Eh-pH diagrams of the system Be-O-H (1) . Eh-pH diagrams of the system Be-O-H (2) . Eh-pH diagrams of the system Bi-O-H . . . Eh-pH diagrams of the system Br-O-H . . . Eh-pH diagrams of the system C-O-H (1) . Eh-pH diagrams of the system C-O-H (2) . Eh-pH diagrams of the system Ca-O-H (1) . Eh-pH diagrams of the system Ca-O-H (2) . Eh-pH diagrams of the system Cd-O-H (1) Eh-pH diagrams of the system Cd-O-H (2) Eh-pH diagrams of the system Ce-O-H (1) . Eh-pH diagrams of the system Ce-O-H (2) . Eh-pH diagrams of the system Cl-O-H . . . Eh-pH diagrams of the system Cm-O-H (1) Eh-pH diagrams of the system Cm-O-H (2) Eh-pH diagrams of the system Co-O-H (1) . Eh-pH diagrams of the system Co-O-H (2) . Eh-pH diagrams of the system Cr-O-H (1) . Eh-pH diagrams of the system Cr-O-H (2) . Eh-pH diagrams of the system Cs-O-H (1) . Eh-pH diagrams of the system Cs-O-H (2) . Eh-pH diagrams of the system Cu-O-H (1) Eh-pH diagrams of the system Cu-O-H (2) Eh-pH diagrams of the system Dy-O-H . . . Eh-pH diagrams of the system Er-O-H . . . Eh-pH diagrams of the system Eu-O-H (1) . Eh-pH diagrams of the system Eu-O-H (2) . Eh-pH diagrams of the system F-O-H (1) . Eh-pH diagrams of the system F-O-H (2) . Eh-pH diagrams of the system Fe-O-H (1) . Eh-pH diagrams of the system Fe-O-H (2) . Eh-pH diagrams of the system Fr-O-H . . . Eh-pH diagrams of the system Ga-O-H . . . Eh-pH diagrams of the system Gd-O-H . . 4

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

8 10 14 15 18 19 22 23 26 27 30 31 33 36 37 40 41 44 45 47 49 52 53 56 57 60 61 64 65 67 70 71 74 75 78 79 82 83 86 87 89 91 94 95 98 99 102 103 105 107 109

52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86 87 88 89 90 91 92 93 94 95 96 97 98 99 100 101 102 103

Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH Eh-pH

diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams diagrams

of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of

the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the

system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system system

Ge-O-H . . . Hf-O-H . . . Hg-O-H (1) . Hg-O-H (2) . Ho-O-H . . . I-O-H (1) . . I-O-H (2) . . In-O-H . . . K-O-H (1) . K-O-H (2) . La-O-H (1) . La-O-H (2) . Li-O-H (1) . Li-O-H (2) . Lu-O-H . . . Mg-O-H (1) Mg-O-H (2) Mn-O-H (1) Mn-O-H (2) Mo-O-H (1) Mo-O-H (2) N-O-H (1) . N-O-H (2) . Na-O-H (1) . Na-O-H (2) . Nb-O-H (1) Nb-O-H (2) Nd-O-H (1) Nd-O-H (2) Ni-O-H (1) . Ni-O-H (2) . Np-O-H (1) Np-O-H (2) Os-O-H . . . P-O-H (1) . P-O-H (2) . Pa-O-H (1) . Pa-O-H (2) . Pb-O-H (1) . Pb-O-H (2) . Pd-O-H . . . Pm-O-H . . Po-O-H . . . Pr-O-H . . . Pt-O-H . . . Pu-O-H (1) . Pu-O-H (2) . Ra-O-H (1) . Ra-O-H (2) . Rb-O-H . . . Re-O-H . . . Rh-O-H . . .

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

111 113 116 117 119 122 123 125 128 129 132 133 136 137 139 142 143 146 147 150 151 154 155 158 159 162 163 166 167 170 171 174 175 177 180 181 184 185 188 189 191 193 195 197 199 202 203 206 207 209 211 213

104 105 106 107 108 109 110 111 112 113 114 115 116 117 118 119 120 121 122 123 124 125 126 127 128 129 130 131 132 133 134 135 136 137 138 139

of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of of

the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the the

Ru-O-H (1) Ru-O-H (2) S-O-H (1) . S-O-H (2) . Sb-O-H (1) . Sb-O-H (2) . Sc-O-H . . . Se-O-H (1) . Se-O-H (2) . Si-O-H (1) . Si-O-H (2) . Sm-O-H (1) Sm-O-H (2) Sn-O-H (1) . Sn-O-H (2) . Sr-O-H (1) . Sr-O-H (2) . Tb-O-H . . . Tc-O-H (1) . Tc-O-H (2) . Te-O-H . . . Th-O-H (1) Th-O-H (2) Tl-O-H . . . Tm-O-H . . U-O-H (1) . U-O-H (2) . V-O-H (1) . V-O-H (2) . W-O-H . . . Y-O-H . . . Yb-O-H . . . Zn-O-H (1) . Zn-O-H (2) . Zr-O-H (1) . Zr-O-H (2) .

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

216 217 220 221 224 225 227 230 231 234 235 238 239 242 243 246 247 249 252 253 255 258 259 261 263 266 267 270 271 273 275 277 280 281 284 285

Introduction

This open file report aims to present an intercomparison of thermodynamic databases by means of EhpH diagrams, which are practical and useful for understanding geochemical behavior of elements. An Eh-pH diagram depicts the dominant aqueous species and stable solid phases on a plane defined by the Eh and pH axes. In an Eh-pH diagram, the solid stability area is related to the saturation condition, and dominant aqueous species give us fundamental information on sorption and colloid phenomena as well as surface characteristics of materials. Eh-pH diagrams are thus essential to understanding solute and radionuclide transport in groundwater. The most well-known studies on comprehensive Eh-pH diagrams are those of Pourbaix (1966) and Brookins (1988). The former discussed corrosion, passivation and immunity of materials, while the latter reported geochemical aspects of the geological disposal of radioactive wastes. These studies have been followed by many thermodynamic databases. With the ever increasing CPU power of computers, we have started utilizing geochemical codes for calculation of complex chemical reactions. Thus, thermodynamic databases have gained importance from a practical perspective. Certain geochemical codes enable us to obtain Eh-pH diagrams easily and quickly. With the aid of software, Eh-pH diagrams can provide us with good insight into the state of the art in thermodynamic databases and the differences between them. It should be noted that this open file report presents the Eh-pH diagrams calculated from databases ”as is”, without any critical comments. It should also be noted that Eh-pH diagrams represent one aspect of thermodynamic databases and databases are often updated, thus this report is only a snapshot of the present. I would be very pleased if this open file report proves useful in helping the readers use thermodynamic databases.

Databases

Let us compare the seven databases listed below. The first database is generic and popular in inorganic chemical engineering. The second and third are generic and popular in geochemistry. The fourth and fifth serve for safety assessment of geological disposal of radioactive wastes, but their coverage of chemical species is sufficiently wide to be suitable for generic use. The sixth and seventh databases mainly cover data on radioactive elements, with incomplete data on other elements. The current report presents only Eh-pH diagrams of radioactive elements included in the sixth and seventh databases. 1. FACT (FACT database) bundled with commercially available software FACTSAGE (FactSage 5.2) (Bale et al., 2002) released by GTT-Technologies. 2. SUPCRT: SUPCRT92 (Johnson et al., 1992) applied with 98 update distributed by Everette Shock from his website on the Internet. 3. Default database “thermo.dat” based on LLNL (Lawrence Livermore National Lab.) data 0.3245r46, bundled with commercially available software GWB (Geochemist’s Workbench) written by C. M. Bethke, Illinois University. 4. JNC-TDB (011213g0 and 011213g2) distributed by Japan Nuclear Cycle Organization from their website (http://migrationdb.jnc.go.jp/). 5. HATCHES (ZZ-HATCHES-15) distributed by NEA (Nuclear Energy Agency) Computer Program Services. 6. Databases tabulated in OECD/NEA Chemical Thermodynamics series 1-4 (Grenthe et al., 1992; Silva et al., 1995; Rard et al., 1999; Lemire et al., 2001). 7. Databases tabulated in OECD/NEA Chemical Thermodynamics series 5 (Guillaumont et al., 2003) which is the updated version of the same series 1-4. 7

List

GWB(Act2)

LLNL JNC-TDB FACT

FactSage(EpH)

SUPCRT HATCHES OECD-NEA OECD-NEAupdate

.bmp

FLASK-AQ

ps2epsi

.ps

Acrobat Distiller

.ps

GWB(Act2)

StarSuite

.eps

.dvi

.ps

printout

template

intermediate file

dvips

LaTeX

Illustrator

.pdf

EhpHdraw

X window graphics

xwd

convert

.xwd

.bmp

Figure 1: Flow chart of creating this report Software is in italics. Dot name represents a ﬁle with format indicated by extention.

Method for constructing Eh-pH diagrams

The present report includes Eh-pH diagrams for the X-H-O system, where X = the symbol of an element like Na, K. This is the most important system for the chemical description of elements in groundwater. To understand the geochemical system of the natural barrier, we took account of not only radioactive elements, but also other elements included in the databases. However, OECD-NEA databases were excluded due to their restricted coverage of the data on non-radioactive elements. Total concentration of elements is 10−10 mole/kg for all diagrams. Such a low concentration enables us to safely assume the activity coeﬃcient to be unity and impedes precipitation of the solid phases which hide the area of dominant aqueous species in the Eh-pH diagram. To avoid unexpected errors during data conversion, databases bundled with commercially available software and databases distributed in the speciﬁc format of the software are handled with appropriate software to draw Eh-pH diagrams. Databases of the former type are FACT and LLNL, bundled with FACTSAGE and GWB, respectively. The database of the latter type is JNC-TDB, which is distributed in three formats: EQ3/6, PHREEQC, and GWB. In this report, a version in the GWB format was used. For the other databases, namely SUPCRT, HATCHES, OECD-NEA, and OECDNEAupdate, the in-house software FLASK-AQ and its companion software EhpHdraw were used to draw the Eh-pH diagrams. The drawing method for Eh-pH diagrams is well explained in many textbooks of chemical thermodynamics (e.g. Garrels and Christ, 1965). The algorithm for drawing Eh-pH diagrams is not documented in the commercially available software FACTSAGE and GWB. FLASK-AQ calculates concentration of aqueous species in equilibrium and moles of stable solid (if present) on grids into which Eh and pH are divided, the Eh in 0.005 V increments from -0.8 V to 1.2 V, the pH in increments of 0.04 from 0 to 14, and outputs the dominant species and the stable solid. Companion program EhpHdraw draws Eh-pH diagrams using the output of FLASK-AQ. This method resembles that reported by Anderko et al. (1997). Unfortunately, since Anderko et al. (1997) did not describe their method in detail, I cannot compare the two methods. The accuracy of the present method for drawing boundaries between dominant species or solids depends on the grid size, which inevitably leads to errors as large as 0.0025 V and 0.02 units for Eh and pH, respectively. The following subsections describe the method for drawing Eh-pH diagrams for each database. The database name and software name (both in abbreviation) are concatenated by a slash (Figure 1).

3.1

FACT/FACTSAGE

Eh-pH diagrams are created with EpH of FACTSAGE and saved as a BMP ﬁle. This ﬁle is used as a template for the line drawing software Illustrator (Adobe Illustrator) and resized to the common axial length.

3.2

SUPCRT/FLASK-AQ

The FLASK-AQ input file was created from the output of SUPCRT92. FLASK-AQ creates an intermediate file from which EhpHdraw draws an Eh-pH diagram on the X window system. This Eh-pH diagram is captured to an X window dump file using ”xwd”, and then converted to a BMP file with ImageMagic. This BMP file is used as a template for Illustrator and resized to the common axial length. An enormous amount of organic species in this database are expressed stoichiometrically in terms of C, H, and O as basis species. Calculations reveal that almost all organic species are decomposed under the stability field of water under ambient conditions.

3.3

LLNL/GWB

The Eh-pH diagram is created with Act2 of GWB and is saved as a PostScript file. This file is converted to a PDF (portable document file) file with Adobe Acrobat Distiller and opened with Illustrator and resized to the common axial length.

3.4

JNC-TDB/GWB

The Eh-pH diagram is created with Act2 of GWB and saved as a PostScript file. This file is converted to a PDF file with Adobe Acrobat Distiller and opened with Illustrator and resized to the common axial length. All diagrams were first created using 011213g0, and S and U data were updated with 011213g2, fixing the erroneous S and U data in the previous version. Visual inspection confirms that all diagrams other than those of S and U are identical between 011213g0 and 011213g2, i.e., that all diagrams from 011213g0 remained unchanged except those of S and U.

3.5

HATCHES/FLASK-AQ

The files of EQ3/6 format data bundled with HATCHES are combined into a single file in which some aux species with the improper keyword ”basis” were corrected. This file is converted to a FLASK-AQ input file using the in-house software AIST TDBCONVERT. FLASK-AQ creates the intermediate file from which EhpHdraw draws an Eh-pH diagram on the X window system. This diagram is captured to an X window dump file using ”xwd”, and then converted to a BMP file with ImageMagic. This BMP file is used as a template for Illustrator and resized to the common axial length. Organic species are expressed stoichiometrically in terms of the ligand species. Note that this method differs from the case of SUPCRT/FLASK-AQ. However, this difference does not affect the Eh-pH diagrams because ligand species are not included in the X-H-O system.

3.6

OECD/NEA

The tables listing the Standard Gibbs Free Energy of formation for the elements in the OECD-NEA Chemical Thermodynamics vol. 1-4 are entered into a spread sheet and saved as a text file and converted into FLASK-AQ format using in-house software. FLASK-AQ creates the intermediate file from which EhpHdraw draws the Eh-pH diagram in the X window system. This Eh-pH diagram is captured to an X window dump file using ”xwd”, and then converted into a BMP file with ImageMagic. This BMP file is used as a template for Illustrator and resized to the common axial length.

Symbol

Database

Ac (JNC-TDB/GWB)

Software

1.2

1.0

0.8

0.6

Stability field of water (298.15K, 105 Pa)

Eh(V)

0.4 AcOH[2+] 0.2

Ac[3+]

Ac(OH)2[+] Ac(OH)3(c)

0.0

Solid phase in bold

-0.2

-0.4

-0.6

-0.8 1

Figure 2: Legend of Eh-pH diagram

3.7

OECD-NEA update

The source database of OECD-NEA Chemical Thermodynamics vol. 5 was processed in the same way as OECD/NEA described above.

Explanation of the diagrams and tables

Tables and diagrams are presented in alphabetical order of the chemical symbol of the element. The tables precede the diagrams for each element. The top row of the table contains the database name. The database name and software name (both abbreviation) concatenated with a slash (”/”) are found above the diagram next to the chemical symbol of the element (Figure 2). A blank column in the table and NODATA in the diagram mean either ”no data for elements” or ”no data for aqueous species of elements”. The expression of the chemical formula used in the table and diagram is the same as in the source database, namely ”as is”. This was done to abide by the concept of the database compilers. Consequently, it should be noted that the expression for hydration and the solid phase diﬀers between the databases. The expression for the charge has the same style throughout, while the expression for the solid has many variants: ”am” denotes amorphous, ”c” or ”cr” denotes crystalline, ”s” or no index indicates no discrimination for amorphous or crystalline. Some solid phases are labeled with mineral names. FACT database uses ”s1”, ”s2”, ”s3” notation for polymorph phases, and the present report uses the same notation for the diagram from FACT/FACTSAGE. The names of solid phases in the table and diagram are typed in bold face. The area between the two diagonal lines from the upper left to the lower right in the diagram indicates the stability ﬁeld of water at 298.15 K and 105 Pa. The tables list chemical species whose Eh-pH diagrams can be drawn individually for the database. Certain chemical species do not appear in the diagram because they are unstable or no data is available on them. Thus, it is important to consult the table carefully when using the diagrams.

Table 1: List of softwares used Software Acrobat Distiller convert EhpHdraw FactSage FLASK-AQ GWB Illustrator Intel C++ compiler pdvips pLaTeX ps2epsi StarSuite tdbconvert xwd

Version 4.0 5.3.8 1.0 5.2 1.1 4.0 8.0 7.0 5.92b p1.6 tetex 2.0.2 5.2.1 6.0 1.0 X11R6.5

OS Windows 2000 Professional Linux (SuSE 7.3) Linux (SuSE 7.3) Windows 2000 Server Linux (SuSE 7.3) Windows 2000 Server Windows 2000 Professional Linux (SuSE 7.3) Linux (Fedra CORE 2) Linux (Fedra CORE 2) Linux (Fedra CORE 2) Linux (RedHat 9.0) Linux (RedHat 9.0) Linux (SuSE 7.3)

Description conversion from PS to pdf conversion from xwd to bmp X window software for Eh-pH drawing Eh-pH calculation and drawing Eh-pH calculation Eh-pH calculation and drawing ﬁnal drawing of Eh-pH diagrams compiling FLASK-AQ and EhpHdraw conversion from dvi to PS and printing document processing of this report conversion from PS to epsi writing tables of species database ﬁle convert X window dump software

Reliability and uncertainty

The reliability and uncertainty of diagrams depend on the following three factors. 1) Reliability of and error in the data in the databases, 2) Uncertainty of the software used for Eh-pH calculation, 3) Fidelity of the drawing. The error is not mentioned in the databases except the OECD-NEA Chemical Thermodynamics Series. The uncertainty in the commercial softwares for drawing Eh-pH diagrams is not described. The uncertainty in FLASK-AQ depends on grid size, as already mentioned. The ﬁdelity of the drawing is conﬁrmed within the grid size of FLASK-AQ by visual inspection. Thus, the overall error excluding errors stemming from the databases and commercial softwares are within ±0.0025 V for Eh and ±0.02 units for pH.

Description of the softwares and their execution environments

The software used for Eh-pH calculation are GTT-Technologies FactSage 5.2 and Illinois University Geochemist’s Workbench 4.0 and the in-house software AIST FLASK-AQ 1.1. FactSage 5.2 and Geochemist’s Workbench 4.0 are executed under a Microsoft Windows 2000 Server on a Dell PowerEdge 2600 (Xeon 2.4GHz x2 SMP with 4GB memory). FLASK-AQ 1.1 is executed under SuSE Linux 7.3 (kernel 2.4.20) on HIT PC (Pentium4 2.8 GHz with 1GB memory). FLASK-AQ 1.1 was compiled with Intel C++ 7.0 compiler and executed with batch scheduling software LSF 4.2. To obtain the Eh-pH diagrams from the intermediate file of FLASK-AQ 1.1, the in-house software AIST EhpHdraw was used. ZZ-HATCHES-15 data was converted into the FLASK-AQ format using the in-house software AIST TDBCONVERT coded by Nihon sgi. All in-house software of AIST will be released to the general public in the future. To obtain snapshots of the Eh-pH diagram drawn by EhpHdraw, the X Window dump software ”xwd” was used. To convert from the XWD to BMP format, ”convert” of ImageMagic was used. These procedures were carried out under Red Hat Linux 9 or Fedra Core 2 on an IA32 PC. Conversion from the PostScript file to the PDF file was performed with Adobe Acrobat Distiller 4.0. Trace of the template image, resizing and cosmetics of the diagrams, and outputting to the EPS file were performed using Adobe Illustrator 8.0 under Microsoft Windows 2000 Professional on an IA32 PC. The lists of chemical species in the tables were created with Sun StarSuite 6.0 and saved as PostScript files and converted into EPS files with ”ps2epsi” under Fedra Core 2 on an IA32 PC. The final draft of this report was printed out using LaTeX and ”dvips”, on a Laser printer under Fedra

Core 2 on an IA32 PC (Table 1). The names of the software, formats, and hardware are trademarks or registered trademarks and the property of their owners.

References Anderko, A. and Shuler, P.J. (1998) A computational approach to predicting the formation of iron sulďŹ de species using stability diagrams, Computers & Geosciences, 23, 647-658. Bale, C.W., Chartrand, P., Degtrev, S.A. , Eriksson, G., Hack, K., Ben Mahfoud, R., Melancon, J., Pelton, A.D., and Petersen, S. (2002) FactSage thermochemical software and databases, Calphad, 26, 189-228. Brookins, D.G. (1988) Eh-pH diagrams for geochemistry, Springer-Verlag New York, 176p. Garrels, R.M. and Christ, C.L. (1965) Solution, minerals and equilibria, Freeman, Cooper & company, San Francisco, 450p. Johnson, J.W., Oelkers, E.H., and Helgeson, H.C. (1992) SUPCRT92: a software package for calculating the standard molal thermodynamic properties of minerals gases, aqueous species, and reactions from 1 to 5000 bar and 0 to 1000â&#x2014;Ś C, Computers & Geosciences, 18, 899-947. Grenthe, I., Fuger, J., Konings, R.J.M. , Lemire, R.J., Muller, A.B., Nguyen-Trung, C., and Wanner, H. (1992) Chemical Thermodynamics of Uranium (Wanner, H., Forest, I., Nuclear Energy Agency, Organisation for Economic Co-operation, Development eds.), vol. 1, Chemical Thermodynamics, North Holland Elsevier Science Publishers B.V., Amsterdam, 715p. Guillaumont, R., Fanghanel, T., Neck, V., Fuger, J. , Palmer, D.A., Grenthe, I., and Rand, M.H. (2003) Update on the chemical thermodynamics of uranium, neptunium, plutonium, americium and technetium (Mompean, F.J., Illemassene, M., Domenech-Orti, C., and Ben-Said K., Nuclear Energy Agency Data Bank, Organisation for Economic Co-operation, Development eds.), vol. 5 Chemical Thermodynamics, North Holland Elsevier Science Publishers B.V., Amsterdam, 964p. Lemire, R.J., Fuger, J., Nitsche, H., Potter, P.E. , Rand, M.H., Rydberg, J., Spahiu, K., Sullivan, J.C., Ullman, W.J., Vitorge,P., and Wanner, H.(2001) Chemical Thermodynamics of Neptunium and Plutonium (Nuclear Energy Agency Data Bank, Organisation for Economic Co-operation, Development ed.), vol. 4, Chemical Thermodynamics, North Holland Elsevier Science Publishers B.V., Amsterdam. 845p. Pourbaix, M. (1966) Atlas of electrochemical equilibria in aqueous solutions (English edition), Pergamon press, Oxford, 644p. Rard, J.A., Rand, M.H., Anderegg, G., and Wanner, H. (1999) Chemical Thermodynamics of Technetium (Sandino, M.C.A., Osthols, E., Nuclear Energy Agency Data Bank, Organisation for Economic Co-operation, Development eds.), vol. 3, Chemical Thermodynamics, North Holland Elsevier Science Publishers B.V., Amsterdam, 544p. Silva, R.J., Bidoglio, G., Rand, M.H. , Robouch, P.B., Wanner, H., and Puigdomenech, I. (1995) Chemical Thermodynamics of Americium (Nuclear Energy Agency, Organisation for Economic Co-operation, Development ed.), vol. 2, Chemical Thermodynamics, North Holland Elsevier Science Publishers B.V., Amsterdam, 374p.

Table 2: List of Ac species FACT

SUPCRT

LLNL

JNC-TDB Ac[3+], AcOH[2+], Ac(OH)2[+], Ac(OH)3(aq), Ac(OH)3(am), Ac(OH)3(c)

HATCHES Ac[3+], AcOH[2+], Ac(OH)3

Ac (SUPCRT/FLASK-AQ)

Ac (FACT/FACTSAGE)

1.0

0.8

0.6

0.4

0.2

Eh(V)

1.2

Eh(V)

1.2

0.2

NO DATA

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ac ( LLNL/GWB)

Ac (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

NO DATA

AcOH[2+] 0.2

0.0

-0.2

-0.4

-0.6

-0.8

Ac[3+]

Ac(OH)2[+] Ac(OH)3(c)

-0.8 1

Figure 3: Eh-pH diagrams of the system Ac-O-H (1).

Ac = 10−10 , 298.15K, 105 Pa.

Ac (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4

AcOH[2+] Ac[3+]

0.2

0.0 Ac(OH)3 -0.2

-0.4

-0.6

-0.8 1

Figure 4: Eh-pH diagrams of the system Ac-O-H (2).

Ac = 10−10 , 298.15K, 105 Pa.

Table 3: List of Ag species FACT Ag[+], AgOH(aq), Ag(OH)2[-],Ag2O(s), Ag2O2(s), Ag2O3(s), Ag(Native silver)

SUPCRT Ag[2+], Ag[+], AgOH(aq), AgO[-], Ag(Native silver)

LLNL Ag[+], Silver

HATCHES Ag[+], Ag(OH)2[-], AgOH(aq), Ag, Ag2O, Ag2O2, Ag2O3

JNC-TDB Ag[+]

Ag (SUPCRT/FLASK-AQ)

Ag (FACT/FACTSAGE) 1.2

1.2 Ag2O3(s)

1.0

1.0 Ag2O2(s)

0.8

0.6

Ag[+]

AgOH(aq)

AgOH(aq) Ag(OH)2[-]

0.2

Eh(V)

0.4

Eh(V)

0.4

AgO[-]

0.2

0.0

0.0 Ag(s)

Ag(s)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ag (LLNL/GWB)

Ag (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.6 Ag[+] 0.4

Eh(V)

0.4

0.2

Ag[+]

0.2

0.0

-0.2

Ag(s)

-0.4

-0.6

-0.8

-0.8 1

Figure 5: Eh-pH diagrams of the system Ag-O-H (1).

Ag = 10−10 , 298.15K, 105 Pa.

Ag (HATCHES/FLASK-AQ) 1.2 Ag2O3(s) 1.0 Ag2O2(s) 0.8 Ag[+] 0.6

Eh(V)

0.4 Ag(OH)2[-] 0.2

0.0 Ag(s) -0.2

-0.4

-0.6

-0.8 1

Figure 6: Eh-pH diagrams of the system Ag-O-H (2).

Ag = 10−10 , 298.15K, 105 Pa.

Table 4: List of Al species FACT Al[3+], AlO2[-], AlOH[2+], Al(s), AlH3(s), Al2O3(s), Al2O3(s2), Al2O3(s3), Al2O3(s4), Al(OH)3(s), Al2O3(H2O)(s), Al2O3(H2O)(s2), Al2O3(H2O)3(s)

SUPCRT AlO[+], HAlO2(aq), Al[3+], AlO2[-], AlOH[2+], Al2O3(Corundum), AlO(OH)(Diaspore), AlO(OH)(Boehmite), Al(OH)3(Gibbsite), AlO[+], HAlO2(aq)

LLNL Al[3+], Al(OH)2[+], Al(OH)3(aq), Al(OH)4[-] Al13O4(OH)24[7+], Al2(OH)2[4+], Al3(OH)4[5+], AlOH[2+], Boehmite, Corundum, Diaspore, Gibbsite

HATCHES Al[3+], Al(OH)[2+], Al(OH)2[+], Al(OH)3(aq), Al(OH)4[-], Boehmite, Corundum, Diaspore, Gibbsite

JNC-TDB Al[3+], AlOH[2+], Al(OH)2[+], Al(OH)3(aq), Al(OH)4[-], Gibbsite

Al (SUPCRT/FLASK-AQ)

Al (FACT/FACTSAGE) 1.2

1.2

1.0

0.8

0.6

0.4

Al2O3(H2O)(s)

Al[3+]

Eh(V)

0.4

0.2

HAlO2(aq)

0.2 AlOH[2+]

AlOH[2+] 0.0

0.0 AlO2[-]

AlO2[-]

-0.2

-0.4

-0.6

-0.8

-0.8 1

Al (LLNL/GWB) 1.2

1.0

0.8

0.6

Al[3+]

Al(OH)2[+]

AlOH[2+]

Eh(V)

0.4

AlOH[2+]

0.2

Al (JNC-TDB/GWB)

1.2

0.4

0.2

Al(OH)4[-]

0.0

-0.2

-0.4

-0.6

-0.8

Al[3+]

Al(OH)4[-] Al(OH)2[+] AlOH3

-0.8 1

Figure 7: Eh-pH diagrams of the system Al-O-H (1).

Al = 10−10 , 298.15K, 105 Pa.

Al (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6 Al[3+]

Eh(V)

0.4 Al(OH)[2+]

0.2 Al(OH)2[+]

0.0

Al(OH)4[-]

-0.2

-0.4

-0.6

-0.8 1

Figure 8: Eh-pH diagrams of the system Al-O-H (2).

Al = 10−10 , 298.15K, 105 Pa.

Table 5: List of Am species FACT

SUPCRT

Am(s), Am(s2), Am (s3), AmO2(s), Am2O3 (s)

LLNL

JNC-TDB

Am[3+], Am[4+], AmO [+], AmO 2[2+], Am(OH)2[+], Am(OH)3(aq), AmOH[2 +], Am(OH) 3(am), Am(OH)3(c)

Am[3+], AmOH[2+], Am(OH)2[+], Am(OH)3 (aq), Am(OH)3(am), Am(OH)3(c)

HATCHES

OECD-NEA

OECD-NEA update

Am[3+], Am[4+], AmO 2[+], AmO 2[2+], Am (OH)2[+], Am(OH)3(a q), AmOH[2+], Am, A m(OH)3, Am2O3, AmH2, AmO2, Am(OH)3(cr)

Am[4+], Am[2+], Am [3+], AmO2[+], AmO2 [2+], AmOH[2+], Am (OH)2[+], Am(OH)3(a q), Am(c), AmO2(c), Am2O3(c), AmH2(c), A m(OH)3(am), Am(OH)3 (c)

Am[4+], Am[2+], Am [3+], AmO2[+], AmO2 [2+], AmOH[2+], Am (OH)2[+], Am(OH)3(a q), Am(cr), AmO2(c r), Am2O3(cr), AmH2 (cr), Am(OH)3(cr)

Am (FACT/FACTSAGE)

Am (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO AQUEOUS SPECIES DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Am (LLNL/GWB)

Am (JNC-TDB/GWB)

1.2

1.0

1.0 AmO2[+]

0.6

0.4

0.2

Eh(V)

0.8

Eh(V)

0.8

0.2

Am[3+]

Am(OH)2[+] Am(OH)3(c) AmOH[2+]

0.0

AmOH[2+] Am(OH)3(aq)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 9: Eh-pH diagrams of the system Am-O-H (1).

Am = 10−10 , 298.15K, 105 Pa.

Am (OECD-NEA/FLASK-AQ)

Am (HATCHES/FLASK-AQ) 1.2

1.2

AmO2[+]

1.0

AmO2[+]

1.0

0.8

0.8 AmO2(c)

AmO2(s)

0.6

0.6 Am[3+]

Am[3+]

0.4 AmOH[2+]

Eh(V)

0.4

AmOH[2+]

0.2

Am(OH)2[+]

0.2

Am(OH)2[+] 0.0

Am(OH)3(c) 0.0

Am(OH)3(c)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Am (OECD-NEA update/FLASK-AQ) 1.2 AmO2[+]

1.0

0.8 AmO2(cr) 0.6

Eh(V)

0.4 Am[3+]

0.2

AmOH[2+]

0.0 Am(OH)2[+] -0.2

Am(OH)3(cr)

-0.4

-0.6

-0.8 1

Figure 10: Eh-pH diagrams of the system Am-O-H (2).

Am = 10−10 , 298.15K, 105 Pa.

Table 6: List of As species FACT

SUPCRT

LLNL

AsO2[-], AsO4[3-], HAsO2(aq), H2AsO3[], H2AsO4[2-], H2AsO4[-], H3AsO4(aq), AsO[+], As(s), As2O3(s), As2O3(s2), As2O5(s),

AsO2[-], AsO4[3-], HAsO2(aq), H2AsO3[], HAsO4[2-], H2AsO4[-], H3AsO4(aq)

As(OH)4[-], AsH3(aq), AsO4[3-], As(OH)3(aq), AsO2OH[2-], H2AsO4[-], H3AsO4(aq), HAsO4[2-] Arsenolite, As2O5(c), Claudetite

HATCHES As(OH)4[-], H2AsO4[], As(OH)3(aq), AsO[+], AsO4[3-], H3AsO4(aq), HAsO2(aq), HAsO4[2], Arsenolite, As2O5(c), As4O6, Claudetite

JNC-TDB

As (FACT/FACTSAGE)

As (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

H3AsO4(aq)

H3AsO4(aq) 0.6

H2AsO4[-]

0.6 H2AsO4[-]

0.4

Eh(V)

HAsO4[2-]

0.2 AsO4[3-]

HAsO2(aq)

HAsO4[2-] 0.2

0.0

-0.2

-0.4

AsO4[3-]

HAsO2(aq)

-0.4

As(s) H2AsO3[-]

AsO2[-]

-0.6

-0.8

-0.8 1

As (LLNL/GWB)

As (JNC-TDB/GWB)

1.2

1.0

0.8

0.8 H3AsO4(aq)

0.6

0.6 H2AsO4[-]

0.2

0.4 As(OH)3(aq)

Eh(V)

0.4

HAsO4[2-]

0.0

0.2

NO DATA

0.0

AsO4[3-]

-0.2

-0.4

AsH3(aq)

As(OH)4[-]

-0.6

-0.6 AsO2OH[2-]

-0.8

-0.8 1

Figure 11: Eh-pH diagrams of the system As-O-H (1).

As = 10−10 , 298.15K, 105 Pa.

As (HATCHES/FLASK-AQ) 1.2

1.0 H3AsO4(aq) 0.8 H2AsO4[-]

0.6

0.4

Eh(V)

HAsO4[2-]

0.2 AsO4[3-]

0.0 As(OH)3(aq) -0.2

-0.4 As(OH)4[-]

-0.6

-0.8 1

Figure 12: Eh-pH diagrams of the system As-O-H (2).

As = 10−10 , 298.15K, 105 Pa.

Table 7: List of Au species FACT AuO3[3-], HAuO3[2], H2AuO3[-], Au(OH)3(aq), Au2O3(s), Au(OH)3(s), Au(s)

SUPCRT Au[3+], Au[+], Au(Native gold)

LLNL Au[+], Au[3+], Gold

JNC-TDB

Au (FACT/FACTSAGE)

Au (SUPCRT/FLASK-AQ)

1.2

1.2 Au[+]

1.0

Au(OH)3(aq) H2AuO3[-]

0.8

HAuO3[2-]

0.6

0.2

Eh(V)

0.4

Eh(V)

0.4

0.6

Au(s)

0.2

Au(s)

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Au (LLNL/GWB)

Au (JNC-TDB/GWB)

1.2

1.2 Au[+]

0.8

0.6

0.4

0.2

Eh(V)

1.0

Eh(V)

1.0

NO DATA

0.2

Au(s)

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 13: Eh-pH diagrams of the system Au-O-H.

Au = 10−10 , 298.15K, 105 Pa.

Table 8: List of B species FACT

SUPCRT

BO2[-], B(OH)3(aq) BH4[-], BO2[-], B4O7[2-], H2BO3[-], H3BO3(aq), H2BO3(H2O2)[-], HB4O7[-], H2B4O7(aq), H5(BO3)2(H2O2)2[-], B(s), B10H14(s), B2O3(s), HBO2(s), HBO2(s2), HBO2(s3), H3BO3(s), B3H3O3(s), B2(OH)4(s)

LLNL B(OH)3(aq), B(OH)4[-], B2O(OH)5[-], B3O3(OH)4[-], B4O5(OH)4[2-], BH4[], B(OH)3(c,Boric acid)

HATCHES B(OH)3(aq), B4O7[2], BH[4-], H2B4O7(aq), H2BO3[-], HB4O7[-], B2O3, Boric Acid, H3BO3(c), HBO2

JNC-TDB B(OH)3(aq), H2BO3[], B(c), B2O3(c), B(OH)3(c), B(g)

B (FACT/FACTSAGE)

B (SUPCRT/FLASK-AQ)

1.2

1.2 H2BO3(H2O2)[-]

1.0

0.8

0.6

B(OH)3(aq)

0.6

H3BO3(aq)

Eh(V)

0.4

Eh(V)

0.4 BO2[-]

0.2

BO2[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.6 BH4[-]

-0.8

-0.8 1

B (LLNL/GWB)

1.0

0.8

0.6

0.4

0.4 B(OH)3(aq)

Eh(V)

1.2

Eh(V)

B (JNC-TDB/GWB)

1.2

0.2

B(OH)4[-]

0.2

0.0

-0.2

-0.4

-0.6

B(OH)3(aq)

H2BO3[-]

BH4[-] -0.8

-0.8 1

Figure 14: Eh-pH diagrams of the system B-O-H (1).

B = 10−10 , 298.15K, 105 Pa.

1.2

B (HATCHES/FLASK-AQ)

1.0

0.8

0.6

B(OH)3(aq)

Eh(V)

0.4 H2BO3[-] 0.2

0.0

-0.2

-0.4

-0.6 BH[4-] -0.8 1

Figure 15: Eh-pH diagrams of the system B-O-H (2).

B = 10−10 , 298.15K, 105 Pa.

Table 9: List of Ba species FACT Ba[2+], BaOH[+], Ba(s), BaH2(s), BaO(s), BaO2(s), Ba(OH)2(s), Ba(OH)2(H2O)8(s)

SUPCRT Ba[2+], BaOH[+]

LLNL Ba[2+], BaOH[+], Ba(OH)2*8H2O(c), BaO(c)

HATCHES Ba[2+], Ba(OH)[+], Ba(OH)2*8H2O, BaO(c)

JNC-TDB Ba[2+], BaOH[+], Ba(c), BaO(c)

Ba (FACT/FACTSAGE)

Ba (SUPCRT/FLASK-AQ)

1.2

1.2 BaO2(s)

1.0

0.8

0.6

0.4 BaOH[+] Ba[2+]

0.2

Eh(V)

0.4

BaOH[+] 0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ba (LLNL/GWB)

Ba (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Ba[2+]

BaOH[+]

Eh(V)

Ba[2+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Ba[2+]

BaOH[+]

-0.8 1

Figure 16: Eh-pH diagrams of the system Ba-O-H (1).

Ba = 10−10 , 298.15K, 105 Pa.

1.2

Ba (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 Ba[2+] 0.2

0.0 Ba(OH)[+] -0.2

-0.4

-0.6

-0.8 1

Figure 17: Eh-pH diagrams of the system Ba-O-H (2).

Ba = 10−10 , 298.15K, 105 Pa.

Table 10: List of Be species FACT Be[2+], BeO2[2-], Be3(OH)3[3+], Be(s), Be(s2), BeO(s), BeO(s2), Be(OH)2(s), Be(OH)2(s2)

SUPCRT

LLNL

Be[2+], BeO2[2-], BeOH[+], BeO(aq), HBeO2[-]

HATCHES Be[2+], BeOH[+], Be(OH)2(aq), Be(OH)3[-], Be(OH)4[2-], Be2(OH)[3+], Be3(OH)3[3+], Be5(OH)6[4+], Be6(OH)8[4+], Be(OH)2(alpha), Be(OH)2(beta)

JNC-TDB

Be (FACT/FACTSAGE)

Be (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.6 Be[2+]

Be[2+]

Eh(V)

0.4

Eh(V)

0.4

0.2

BeOH[+] BeO(aq)

0.2

Be(OH)2(s2) 0.0

0.0

HBeO2[-]

BeO2[2-] -0.2

-0.2

-0.4

-0.6

-0.8

-0.8 1

Be (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Be (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 18: Eh-pH diagrams of the system Be-O-H (1).

Be = 10−10 , 298.15K, 105 Pa.

1.2

Be (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 Be[2+] 0.2 Be(OH)2(aq) 0.0 Be(OH)3[-] -0.2

-0.4

-0.6

-0.8 1

Figure 19: Eh-pH diagrams of the system Be-O-H (2).

Be = 10−10 , 298.15K, 105 Pa.

Table 11: List of Bi species FACT Bi[3+], BiO[+], BiOH[2+], Bi6O6[6+], Bi6O6(OH)3[3+], Bi9(OH)20[7+], Bi9(OH)21[6+], Bi9(OH)22[5+], Bi(s), Bi2O3(s), Bi2O3(s2), BiOOH(s)

SUPCRT

LLNL

JNC-TDB Bi[3+], BiOH[2+], Bi(OH)2[+], Bi(OH)3(aq), Bi(OH)4[-], Bi6(OH)12[6+], Bi9(OH)20[7+], Bi9(OH)21[6+], Bi9(OH)22[5+], Bi3(OH)4[5+] Bi(c), Bi2O3(s)

Bi[3+], BiO[+], BiOH[2+], HBiO2(aq), BiO2[-]

Bi (FACT/FACTSAGE) 1.2

1.0

0.8

Bi[3+]

0.8

0.6

0.4

Eh(V)

Bi (SUPCRT/FLASK-AQ)

1.2

BiO[+] 0.2

BiOOH(s)

0.0

Bi[3+]

BiOH[2+] BiO[+]

0.2 HBiO2(aq)

0.0

-0.2

-0.2 BiO2[-]

Bi(s) -0.4

-0.4

-0.6

-0.8

-0.8 1

Bi (LLNL/GWB)

Bi (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

BiOH[2+]

Eh(V)

Bi[3+]

NO DATA

0.2

Bi(OH)2[+]

Bi(OH)3(aq) Bi(OH)4[-]

0.2

0.0

-0.2

-0.4

-0.4 Bi(c)

-0.6

-0.8

-0.8 1

Figure 20: Eh-pH diagrams of the system Bi-O-H.

Bi = 10−10 , 298.15K, 105 Pa.

Table 12: List of Br species FACT Br[-], Br2(aq), Br3[-], Br5[-], BrO[-], BrO3[-], HBrO(aq)

SUPCRT Br[-], Br3[-], BrO[-], BrO3[-], HBrO(aq), BrO4[-]

LLNL Br[-]

JNC-TDB Br[-], Br2(aq), Br2(l), BrO[-], BrO3[-], HBrO(aq), Br(g), Br2(g), HBr(g)

Br (FACT/FACTSAGE)

Br (SUPCRT/FLASK-AQ)

1.2

1.2 BrO4[-]

1.0

0.8

0.6

0.4

Eh(V)

BrO3[-]

Br[-]

0.2

Br[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Br (LLNL/GWB)

Br (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

BrO3[-]

Br2(l) 0.4

Eh(V)

0.4

Br[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Br[-]

-0.8 1

Figure 21: Eh-pH diagrams of the system Br-O-H.

Br = 10−10 , 298.15K, 105 Pa.

Table 13: List of C species (1) FACT

SUPCRT

LLNL

JNC-TDB

CH4(aq), C2H2(aq), C2H4(aq), C2H6(aq), CO(aq), CO2(aq), CO3[2-], C2O4[2-], CH3OH(aq), C2H5O[-], CH3CH2OH(aq), HCOO[-], HCOOH(aq), CH3COO[-], CH3COOH(aq), HCO3[], HC2O4[-], C(s), C(s2)

CH4(aq,Methan), C2H2 (aq,Ethyne), C2H4(aq,Ethylene), C2H6(aq,Ethane), CO(aq), CO2(aq), CO3[2-], C2O4[2-] (Oxalate), CH3OH(aq,Methanol), C2H5OH(aq,Ethanol), HCO2[-](Formate), H2CO2(aq, Formicacid), C2H3O2[-] (Acetate), C2H4O2(aq,Aceticacid), HCO3[-], C2HO4[-](HOxalate), C4H9OH (aq,1-Butanol), C4H8(aq,1-Butene), C4H6(aq,1-Butyne), C7H15OH (aq,1-Heptanol), C7H14(aq,1-Heptene), C7H12(aq,1-Heptyne), C6H13OH(aq,1Hexanol), C6H12(aq, 1-Hexene), C6H10(aq, 1-Hexyne), C8H17OH(aq,1Octanol), C8H16(aq, 1-Octene), C8H14(aq, 1-Octyne), C5H11OH(aq,1Pentanol), C5H10(aq, 1-Pentene), C5H8(aq, 1-Pentyne), C3H7OH(aq,1Propanol), C3H6 (aq, 1-Propene), C3H4(aq, 1-Propyne), C4H8O(aq,2Butanone), C7H14O (aq,2-Heptanone), C6H12O(aq,2Hexanone), C4H7O3[](2Hydroxybutanoate), C4H8O3(aq,2Hydroxybutanoic), C10H19O3[-] (2Hydroxydecanoate), C10H20O3(aq,2Hydroxydecanoic), C7H13O3[-](2Hydroxyheptanoate), C7H14O3(aq,2Hydroxyheptanoic), C6H11O3[-](2Hydroxyhexanoate), C6H12O3(aq,2Hydroxyhexanoic), C9H17O3[-](2Hydroxynonanoate), C9H18O3(aq,2Hydroxynonanoic),

HCO3[-], (Ophth)[2-], CH3COO[], CH4(aq), CO2(aq), CO3[2-], H(O-phth)[-], H2(Ophth), HCH3COO, Graphite, O-phth acid(c), CH4(g), CO2(g)

CO3[2-], CH4(aq), HCO3[-], CO2(aq), C(c), CH4(g), C(g), CO(g), CO2(g)

Table 14: List of C species (2) C (CONTINUED) FACT

SUPCRT

LLNL

C8H15O3[-](2Hydroxyoctanoate), C8H16O3(aq,2Hydroxyoctanoic), C5H9O3[-](2Hydroxypentanoate), C5H10O3(aq,2Hydroxypentanoic), C8H16O(aq,2Octanone), C5H10O(aq,2Pentanone), C3H6O (aq,Acetone), C6H8O4[2-] (Adipate), C6H10O4 (aq,Adipic-acid), C9H16O4 (aq,Azelaicacid), C9H14O4[2-] (Azelate), C6H6(aq, Benzene), C7H5O2[-] (Benzoate), C7H6O2(aq,Benzoicacid), C4H10(aq, Butane), C4H8O2(aq, Butanoic-acid), C6H4OHCH3(aq,oCresol), C6H4OHCH3(aq,mCresol), C6H4OHCH3(aq,pCresol), C10H19O2[-] (Decanoate), C10H20O2(aq,Decanoicacid), C6H3OHCH3CH3(aq, 2-3DMP), C6H3OHCH3CH3(aq, 2-4DMP), C6H3OHCH3CH3(aq, 2-5DMP), C6H3OHCH3CH3(aq, 2-6DMP), C6H3OHCH3CH3(aq, 3-4DMP), C6H3OHCH3CH3(aq, 3-5DMP), C12H23O2[-] (Dodecanoate), C12H24O2 (aq,Dodecanoicacid), CH3COOCH2CH3(aq, Ethylacetate), C6H5C2H5(aq, Ethylbenzene), C5H6O4[2](Glutarate), C5H8O4 (aq,Glutaric-acid), C2H3O3[](Glycolate), C2H4O3 (aq,Glycolic-acid), C6H9O4[-](HAdipate), C9H15O4[-] (H-Azelate),

JNC-TDB

C (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.4

CO2(aq)

0.2

Eh(V)

C (SUPCRT/FLASK-AQ)

1.2

HCO3[-]

0.0

CO2(aq)

0.2

HCO3[-] CO3[2-]

0.0

CO3[2-]

-0.2

-0.4

CH4(aq)

-0.4

H-SUCCINATE(aq)

-0.6

HEPTANOATE(aq)

CH4(aq) -0.6

-0.8

-0.8 1

C (LLNL/GWB)

C (JNC-TDB/GWB)

1.2

1.0

0.8

0.8 CO2(aq)

0.6

CO2(aq)

HCO3[-] HCO3[-]

0.4

CO3[2-]

Eh(V)

0.4

0.2

0.0

-0.2

-0.4

CO3[2-]

0.2

-0.4 CH4(aq)

CH4(aq) -0.6

-0.6

-0.8

-0.8 1

Figure 22: Eh-pH diagrams of the system C-O-H (1).

C = 10−10 , 298.15K, 105 Pa.

C (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6 H2CO3(aq)

Eh(V)

0.4 HCO3[-]

0.2

0.0

CO3[2-]

-0.2 CH4(aq) -0.4

-0.6

-0.8 1

Figure 23: Eh-pH diagrams of the system C-O-H (2).

C = 10−10 , 298.15K, 105 Pa.

Table 15: List of Ca species FACT

SUPCRT

Ca[2+], CaOH[+], Ca[2+], CaOH[+], Ca(s), Ca(s2), CaO(Lime) CaH2(s), CaO2(s), Ca(OH)2(s), CaO(s)

LLNL Ca[2+], CaOH[+], Ca(OH)2(c), Lime, Portlandite

JNC-TDB Ca[2+], CaOH[+], CaO(s, Lime_qu), Ca(c), CaO(c), Ca(g)

HATCHES Ca[2+], Ca(OH)[+], Ca(OH)2, CaO Remarks JNC-TDB: Detailed description of Lime_qu is not given, it may be lime quenched?

Ca (FACT/FACTSAGE)

Ca (SUPCRT/FLASK-AQ)

1.2

1.2 CaO2(s)

0.8

0.6

0.4

Eh(V)

1.0

Eh(V)

1.0

Ca[2+]

0.2

Ca[2+] CaOH[+]

CaOH[+] 0.0

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ca (LLNL/GWB)

Ca (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

0.2

Ca[2+]

Eh(V)

1.2

Eh(V)

1.2

0.2

CaOH[+]

0.0

-0.2

-0.4

-0.6

-0.8

Ca[2+]

CaOH[+]

-0.8 1

Figure 24: Eh-pH diagrams of the system Ca-O-H (1).

Ca = 10−10 , 298.15K, 105 Pa.

Ca (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4 Ca[2+] 0.2

0.0 Ca(OH)[+] -0.2

-0.4

-0.6

-0.8 1

Figure 25: Eh-pH diagrams of the system Ca-O-H (2).

Ca = 10−10 , 298.15K, 105 Pa.

Table 16: List of Cd species FACT

SUPCRT

LLNL

Cd[2+], CdO2[2-], Cd[2+], CdO2[2-], CdOH[+], HCdO2[-], CdOH[+], HCdO2[-], Cd(OH)2(aq), Cd(s), CdO(aq) CdO(s), Cd(OH)2(s)

HATCHES Cd[2+], Cd(OH)2(aq), Cd(OH)3[-], Cd(OH)4[2-], Cd2OH[3+], Cd4(OH)4[4+], CdOH[+], Cd(OH)2

JNC-TDB

Cd (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.4

Cd[2+]

0.4

Cd[2+]

0.2

Eh(V)

Cd (SUPCRT/FLASK-AQ)

1.2

CdOH[+]

0.2

CdOH[+] Cd(OH)2(aq)

CdO(aq)

0.0

0.0 HCdO2[-] CdO2[2-]

-0.2

-0.4

-0.6

-0.6 Cd(s)

-0.8 1

HCdO2[-]

-0.8 9

Cd (LLNL/GWB)

Cd (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 26: Eh-pH diagrams of the system Cd-O-H (1).

Cd = 10−10 , 298.15K, 105 Pa.

Cd (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4 Cd[2+] 0.2 Cd(OH)[+] 0.0 Cd(OH)2(aq)

-0.2

Cd(OH)3[-]

-0.4

-0.6

-0.8 1

Figure 27: Eh-pH diagrams of the system Cd-O-H (2).

Cd = 10−10 , 298.15K, 105 Pa.

Table 17: List of Ce species FACT Ce[3+], Ce[4+], Ce(s), Ce(s2), CeH2(s), CeO2(s), Ce2O3(s), Ce6O11(s), Ce18O31(s)

SUPCRT

LLNL

Ce[3+], Ce[4+], Ce[2+], CeOH[2+], CeO[+], CeO2H (aq), CeO2[-]

HATCHES Ce[3+], Ce2(OH)2[4+], Ce3(OH)5[4+], CeOH[2+], Ce(OH)3, Ce2O3

JNC-TDB

Ce (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.4 CeO2(s)

Ce[3+]

0.2

Eh(V)

Ce (FACT/FACTSAGE) 1.2

0.0

Ce[3+] 0.2 CeO[+]

0.0

CeO2H(aq) -0.2

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ce (LLNL/GWB)

Ce (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

CeO2[-]

0.2

NO DATA

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 28: Eh-pH diagrams of the system Ce-O-H (1).

Ce = 10−10 , 298.15K, 105 Pa.

1.2

Ce (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4

Ce[3+]

0.2 CeOH[2+] 0.0 Ce(OH)3(s)

-0.2

-0.4

-0.6

-0.8 1

Figure 29: Eh-pH diagrams of the system Ce-O-H (2).

Ce = 10−10 , 298.15K, 105 Pa.

Table 18: List of Cl species FACT Cl2(aq), Cl3[-], ClO2(aq), Cl[-], ClO[-], ClO2[-], ClO4[-], ClO3[-], HOCl(aq), HClO2(aq)

SUPCRT Cl[-], ClO[-], ClO2[-], ClO3[-], ClO4[-], HClO(aq), HClO2(aq), HCl(aq)

LLNL Cl[-], ClO4[-], HCl(aq)

JNC-TDB Cl[-], ClO[-], ClO2[-], ClO3[-], ClO4[-], HClO(aq), HClO2(aq), Cl(g), Cl2(g), HCl(g)

Cl (FACT/FACTSAGE)

Cl (SUPCRT/FLASK-AQ)

1.2

1.0

ClO4[-]

0.8

0.6

0.4

0.2

Eh(V)

1.0

Cl[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Cl[-]

-0.8 1

Cl (LLNL/GWB)

Cl (JNC-TDB/GWB)

1.2

1.0

ClO4[-]

0.8

0.6

0.4

0.2

Eh(V)

ClO4[-]

Cl[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

ClO4[-]

Cl[-]

-0.8 1

Figure 30: Eh-pH diagrams of the system Cl-O-H.

Cl = 10−10 , 298.15K, 105 Pa.

Table 19: List of Cm species FACT

SUPCRT

LLNL

JNC-TDB Cm[3+], CmOH[2+], Cm(OH)2[+], Cm(OH)3(aq), Cm(OH)3(am), Cm(OH)3(c)

HATCHES Cm[3+], Cm[4+], Cm(OH)[2+], Cm(OH)2[+], Cm(OH)3, Cm2O3, CmO2

Cm (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Cm (FACT/FACTSAGE) 1.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Cm (JNC-TDB/GWB)

Cm (LLNL/GWB) 1.2

1.2

1.0

0.8

0.6

0.4

Eh(V)

NO DATA

0.2 NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Cm[3+]

Cm(OH)2[+] CmOH[2+]

Cm(OH)3(c)

-0.8 1

Figure 31: Eh-pH diagrams of the system Cm-O-H (1).

Cm = 10−10 , 298.15K, 105 Pa.

1.2

Cm (HATCHES/FLASK-AQ) CmO2(s)

1.0

0.8

0.6

Eh(V)

0.4 Cm[3+]

0.2

Cm(OH)[2+] Cm(OH)2[+]

0.0

Cm(OH)3(s)

-0.2

-0.4

-0.6

-0.8 1

Figure 32: Eh-pH diagrams of the system Cm-O-H (2).

Cm = 10−10 , 298.15K, 105 Pa.

Table 20: List of Co species FACT Co[2+], Co[3+], HCoO2[-], Co(OH)2(aq), Co(s), Co(s2), CoO(s), Co3O4(s), Co(OH)2(s)

SUPCRT Co[2+], Co[3+], HCoO2[-], CoO(aq), CoOH[+], CoO2[2-], CoOH[2+]

LLNL Co[2+], Co[3+], Co(OH)2(aq), Co(OH)3[-], Co(OH)4[2-], Co2(OH)3[+], Co4(OH)4[4+], CoOH[+], HCoO2[-], Co(OH)2(s,pink), Co3O4, CoO

HATCHES Co[2+], Co[3+], Co(OH)2(aq), Co(OH)3[-], Co(OH)4[2-], Co2OH[3+], Co4(OH)4[4+], CoOH[+], Co(OH)2, Co3O4, CoO

JNC-TDB Co[2+], CoO(s, COBALTO2)

Co (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Co (FACT/FACTSAGE) 1.2

Co(OH)2(aq)

0.2

Co[2+]

0.0

-0.2

-0.4

-0.6

-0.8

HCoO2[-]

0.2

CoO(aq)

-0.8 1

Co (LLNL/GWB)

Co (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Co3O4(s) 1.0

Co[2+]

0.2

Co[2+]

COBALTO2(s)

HCoO2[-] 0.0

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 33: Eh-pH diagrams of the system Co-O-H (1).

Co = 10−10 , 298.15K, 105 Pa.

Co (HATCHES/FLASK-AQ) 1.2

1.0 Co3O4(s)

0.8

0.6 Co[2+]

Eh(V)

0.4

0.2 Co(OH)2(aq)

0.0

Co(OH)3[-]

-0.2

-0.4

-0.6

-0.8 1

Figure 34: Eh-pH diagrams of the system Co-O-H (2).

Co = 10−10 , 298.15K, 105 Pa.

Table 21: List of Cr species FACT

SUPCRT

LLNL

Cr[2+], Cr[3+], CrO4[2-], Cr2O7[2-], CrOH[2+], HCrO4[-], Cr(s), CrO2(s), CrO3(s), Cr2O3(s), Cr3O4(s), Cr5O12(s), Cr8O21(s)

Cr[2+], Cr[3+], CrO4[2-], Cr2O7[2-], CrOH[2+], HCrO4[-], HCrO2(aq), CrO2[-], CrO[+]

Cr[3+], Cr[2+], CrO4[2-], CrO4[3-], Cr(OH)2[+], Cr(OH)3(aq), Cr(OH)4[-], Cr2(OH)2[4+], Cr2O7[2-], Cr3(OH)4[5+], CrOH[2+], H2CrO4(aq), HCrO4[], Cr2O3(s), CrO2(s), CrO3(s)

HATCHES Cr[3+], Cr[2+], CrO4[2-], Cr(OH)2[+], Cr(OH)3(aq), Cr(OH)4[-], Cr2(OH)2[4+], Cr2O7[2-], Cr3(OH)4[4+], CrOH[2+], H2CrO4(aq), HCrO4[], Cr(OH)3, Cr2O3, CrO2

JNC-TDB

Cr (FACT/FACTSAGE)

Cr (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 HCrO4[-]

0.8

HCrO4[-]

0.8

0.6

0.6 Cr[3+] 0.4

CrO4[2-]

Eh(V)

0.4

0.2 CrOH[2+]

0.0

Cr[3+]

CrO4[2-]

0.2

CrOH[2+]

0.0 Cr2O3(s)

-0.2

CrO[+] HCrO2(aq)

-0.2

CrO2[-] -0.4

-0.4

-0.6

Cr[2+]

-0.8

-0.8 1

Cr (LLNL/GWB) 1.2

1.0

1.0 HCrO4[-]

0.8

0.6

0.6 CrO4[2-]

0.4

Eh(V)

0.4

Eh(V)

Cr (JNC-TDB/GWB)

1.2

0.2

Cr[2+]

Cr[3+]

0.2

NO DATA

CrOH[2+] 0.0

0.0 CrO4[3-]

-0.2

-0.2 Cr2O3(s)

-0.4

-0.6

Cr(OH)4[-]

-0.6

Cr[2+] -0.8

-0.8 1

Figure 35: Eh-pH diagrams of the system Cr-O-H (1).

Cr = 10−10 , 298.15K, 105 Pa.

1.2

Cr (HATCHES/FLASK-AQ) HCrO4[-]

1.0

CrO4[2-] 0.8

0.6 Cr[3+]

Eh(V)

0.4

0.2

0.0 Cr2O3(s) -0.2

-0.4

-0.6

Cr[2+]

-0.8 1

Figure 36: Eh-pH diagrams of the system Cr-O-H (2).

Cr = 10−10 , 298.15K, 105 Pa.

Table 22: List of Cs species FACT Cs[+], Cs(s), CsO2(s), Cs2O(s), Cs2O3(s), CsOH(s), CsOH(s2), CsOH(s3)

SUPCRT Cs[+], CsOH(aq)

LLNL Cs[+]

HATCHES Cs[+], CsO, CsOH

JNC-TDB Cs[+], Cs(c), Cs2O(s), CsOH(s), Cs(g)

Cs (FACT/FACTSAGE)

Cs (SUPCRT/FLASK-AQ)

1.2

1.2 CsO2(s)

1.0

0.8

0.6

0.4

Eh(V)

1.0

Cs[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Cs (LLNL/GWB)

Cs (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Cs[+]

0.2

Cs[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Cs[+]

0.2

-0.8 1

Figure 37: Eh-pH diagrams of the system Cs-O-H (1).

Cs = 10−10 , 298.15K, 105 Pa.

1.2

Cs (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4

0.2

Cs[+]

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 38: Eh-pH diagrams of the system Cs-O-H (2).

Cs = 10â&#x2C6;&#x2019;10 , 298.15K, 105 Pa.

Table 23: List of Cu species FACT Cu[+], Cu[2+], CuO2[2-], HCuO2[-], Cu(OH)2(s), Cu (s), CuO(s), Cu2O(s)

SUPCRT

LLNL

Cu[+], Cu[2+], Cu[+], Cu[2+], CuO2[2-], HCuO2[-], CuOH[+], Copper, Cuprite, Tenorite CuOH[+], CuO(aq), Cu(Native Copper), CuO(Tenorite), Cu2O (Cuprite)

HATCHES Cu[2+], Cu[+], Cu(OH)4[2-], Cu2(OH)2[2+], Copper, Cuprite, Tenorite

JNC-TDB

Cu (FACT/FACTSAGE)

Cu (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

Cu[2+]

0.6

Cu(OH)2(s)

0.4

Eh(V)

0.4

HCuO2[-]

0.2

CuO2[2-]

Cu[+]

0.0

Cu[2+]

CuO(aq) CuO2[2-]

0.2

HCuO2[-]

Cu[+]

0.0

Cuprite

Cu2O(s) -0.2

-0.2 Cu(s)

Cu(s)

-0.4

-0.6

-0.8

-0.8 1

Cu (LLNL/GWB)

Cu (JNC-TDB/GWB)

1.2

1.0

0.8

0.8 Cu[2+]

0.6

0.6 CuOH[+] 0.4

Eh(V)

0.4 Tenorite 0.2 Cu[+]

0.0

NO DATA

0.2

0.0 Cuprite

-0.2

Copper -0.4

-0.4

-0.6

-0.8

-0.8 1

Figure 39: Eh-pH diagrams of the system Cu-O-H (1).

Cu = 10−10 , 298.15K, 105 Pa.

1.2

Cu (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Cu[2+]

0.4

Eh(V)

Tenorite

0.2

Cu(OH)4[2-] Cu[+]

0.0

Cuprite -0.2 Copper -0.4

-0.6

-0.8 1

Figure 40: Eh-pH diagrams of the system Cu-O-H (2).

Cu = 10−10 , 298.15K, 105 Pa.

Table 24: List of Dy species FACT Dy[3+], Dy(s), Dy(s2), Dy2O3(s)

SUPCRT

LLNL

Dy[3+], Dy[2+], Dy[4+], DyOH[2+], DyO[+], DyO2H(aq), DyO2[-]

JNC-TDB

Dy (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.4 Dy[3+]

0.2

Eh(V)

Dy (FACT/FACTSAGE) 1.2

Dy2O3(s)

Dy[3+] DyOH[2+]

0.2

DyO[+] DyO2[-]

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Dy (JNC-TDB/GWB)

Dy (LLNL/GWB) 1.2

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

NO DATA

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 41: Eh-pH diagrams of the system Dy-O-H.

Dy = 10−10 , 298.15K, 105 Pa.

Table 25: List of Er species FACT Er[3+], Er(s), Er2O3(s), Er2O3(s2)

SUPCRT

LLNL

Er[3+], Er[2+], Er[4+], ErOH[2+], ErO[+], ErO2H(aq), ErO2[-]

JNC-TDB

Er (SUPCRT/FLASK-AQ)

Er (FACT/FACTSAGE) 1.2

1.2

1.0

0.8

0.6

0.4 Er[3+]

Er2O3(s)

Eh(V)

0.4

0.2

Er[3+] ErOH[2+]

0.2

ErO[+] 0.0

0.0 ErO2[-]

-0.2

-0.4

-0.6

-0.8

-0.8 1

Er (JNC-TDB/GWB)

Er (LLNL/GWB) 1.2

1.2

1.0

0.8

0.6

0.4

Eh(V)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 42: Eh-pH diagrams of the system Er-O-H.

Er = 10−10 , 298.15K, 105 Pa.

Table 26: List of Eu species FACT Eu[2+], Eu[3+], Eu(s), EuH2(s), EuO(s), Eu2O3(s), Eu2O3(s2), Eu3O4(s), EuO3H3(s)

SUPCRT Eu[2+], Eu[3+], Eu[4+], EuOH[2+], EuO[+], EuO2H(aq), EuO2[-]

LLNL Eu[3+], Eu[2+], Eu(OH)2[+], EuOH[2+], Eu(s), Eu(OH)3(s), Eu2O3(cubic), Eu2O3(monoclinic), Eu3O4(s), EuO(s)

HATCHES Eu[3+], Eu(OH)[2+], Eu, Eu(OH)3, Eu2O3(cubic), Eu2O3(monoclinic), Eu3O4, EuO

JNC-TDB

Eu (FACT/FACTSAGE)

Eu (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4 EuO3H3(s)

Eu[3+]

Eh(V)

0.4

0.2

0.0

Eu[3+]

0.2 EuOH[2+] EuO[+]

0.0

EuO2[-] -0.2

-0.2

-0.4

Eu[2+]

-0.6

-0.8

-0.8 1

Eu (LLNL/GWB) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Eu[3+] Eu(OH)2[+] Eu(OH)3(s)

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

Eu (JNC-TDB/GWB)

1.2

0.4

Eh(V)

Eu[2+]

-0.6

Eu[2+]

-0.8

-0.8 1

Figure 43: Eh-pH diagrams of the system Eu-O-H (1).

Eu = 10−10 , 298.15K, 105 Pa.

Eu (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Eu[3+]

0.2 Eu(OH)[2+]

0.0

Eu(OH)3(s)

-0.2

-0.4

-0.6

-0.8 1

Figure 44: Eh-pH diagrams of the system Eu-O-H (2).

Eu = 10−10 , 298.15K, 105 Pa.

Table 27: List of F species FACT

SUPCRT

LLNL

F[-], HF(aq), HF2[-] F[-], HF(aq), HF2[-] F[-], H2F2, HF, HF2[-]

HATCHES F[-], HF(aq), HF2[-]

JNC-TDB F-, HF(aq), HF2[-], F(g), F2(g), HF(g)

F (FACT/FACTSAGE)

F (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4 F[-]

HF(aq)

Eh(V)

0.4

0.2

HF(aq) 0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

F (LLNL/GWB) 1.2

1.0

0.8

0.6

0.4

0.2

F (JNC-TDB/GWB)

1.2

Eh(V)

F[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

HF(aq)

F[-]

-0.8 1

Figure 45: Eh-pH diagrams of the system F-O-H (1).

F = 10−10 , 298.15K, 105 Pa.

1.2

F (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 HF(aq)

0.2 F[-] 0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 46: Eh-pH diagrams of the system F-O-H (2).

F = 10−10 , 298.15K, 105 Pa.

100

Table 28: List of Fe species FACT Fe[2+], Fe[3+], FeOH[+], FeOH[2+], HFeO2[-], Fe(OH)2[+],FeO2[2], Fe(OH)3(aq), Fe2(OH)2[4+], Fe(s), Fe(s2), Fe2O3(s2), Fe2O3(s3), Fe3O4(s2), Fe3O4(s3), Fe3O4(s4), Fe(OH)2(s), Fe(OH)3(s), Fe2O3(H2O)(s), FeO (s), Fe2O3(s), Fe3O4(s)

SUPCRT HFeO2(aq), FeO2[-], FeO(aq), Fe[2+], Fe[3+], FeOH[+], FeOH[2+], HFeO2[-], FeO[+], FeO (Ferrous-oxide), Fe2O3(Hematite), Fe3O4(Magnetite)

LLNL Fe[2+], Fe[3+], Fe(OH)2(aq), Fe(OH)2[+], Fe(OH)3(aq), Fe(OH)3[-], Fe(OH)4[-], Fe2(OH)2[4+], Fe3(OH)4[5+], FeOH[+], FeOH[2+], Fe(OH)2(ppd), Fe(OH)3(ppd), FeO(c) Goethite, Hematite, Magnetite, Wustite

HATCHES Fe[2+], Fe[3+], Fe(OH)[+], Fe(OH)2(aq), Fe(OH)2[+], Fe(OH)3(aq), Fe(OH)3[-], Fe(OH)4[-], Fe(OH)4[2-], Fe2(OH)2[4+], Fe3(OH)4[5+], FeOH[2+], Fe(OH)2, Fe(OH)3, FeO(c), Goethite, Hematite, Magnetite, Wustite

101

JNC-TDB Fe[2+], Fe[3+], FeOH[2+], Fe(OH)2[+], Fe(OH)3(aq), FeOH4[-], Fe2(OH)2[4+], Fe3(OH)4[5+], FeOH[+], Fe(OH)2(aq), Fe(OH)3[-], Fe(OH)3(a) Hematite, Magnetite, Goethite

Fe (SUPCRT/FLASK-AQ)

Fe (FACT/FACTSAGE) 1.2

1.0

1.2

1.0

Fe[3+]

Fe[3+] FeOH[2+]

FeOH[2+] 0.8

0.8

0.6

FeO[+]

Fe2O3(s) 0.4

Eh(V)

0.4 Fe2O3(s)

0.2

Fe[2+]

0.0

-0.2

-0.4

FeO2[-]

0.2

-0.4

FeOH[+]

Fe3O4(s) -0.6

HFeO2[-]

-0.6 HFeO2[-] Fe(s)

-0.8 1

-0.8

Fe (LLNL/GWB)

1.2

1.0

Fe[3+]FeOH[2+]

Fe[3+] FeOH[2+]

Fe(OH)2[+]

0.8

0.6

0.6 Hematite

Hematite 0.4

Eh(V)

0.4

Eh(V)

Fe (JNC-TDB/GWB)

1.2

1.0

Fe(OH)4[-] Fe[2+]

0.2

FeOH4[-] Fe[2+]

0.2

0.0

-0.2

-0.2 Magnetite

-0.4

Magnetite

-0.6

Fe(OH)3[-]

FeOH[+]

FeO(c)

-0.8 1

-0.6 FeOH3[-]

FeOH[+] -0.8

Figure 47: Eh-pH diagrams of the system Fe-O-H (1).

102

Fe = 10−10 , 298.15K, 105 Pa.

1.2

Fe (HATCHES/FLASK-AQ)

1.0 Fe[3+] FeOH[2+] 0.8

Fe(OH)2[+]

0.6

0.4

Eh(V)

Hematite

0.2 Fe[2+]

0.0

Fe(OH)4[-]

-0.2

Magnetite

-0.4

-0.6

Fe(OH)3[-]

-0.8 1

Figure 48: Eh-pH diagrams of the system Fe-O-H (2).

103

Fe = 10−10 , 298.15K, 105 Pa.

Table 29: List of Fr species FACT

SUPCRT

LLNL

Fr[+]

104

JNC-TDB

Fr (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Fr (FACT/FACTSAGE) 1.2

NO DATA

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Fr (LLNL/GWB)

Fr (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Fr[+]

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 49: Eh-pH diagrams of the system Fr-O-H.

105

Fr = 10−10 , 298.15K, 105 Pa.

Table 30: List of Ga species FACT

SUPCRT

LLNL

Ga[3+], GaOH[2+], Ga[3+], GaOH[2+], Ga(OH)2[+], H2GaO3[- GaO[+], GaO2[-], ],Ga[2+], GaO3[3-], HGaO2(aq) HGaO2[2-], Ga(s), Ga2O3(s), Ga(OH)3(s)

106

JNC-TDB

Ga (FACT/FACTSAGE)

Ga (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 Ga[3+] GaOH[2+]

0.8

Ga2O3(s) H GaO [-] 2 3 0.8

GaO3[3-]

Ga(OH)2[+]

0.6

0.6 Ga[3+] GaOH[2+]

0.4

Eh(V)

0.4

HGaO2[2-]

0.2

GaO[+]

0.0

-0.2

-0.4

-0.6

-0.8

HGaO2(aq)

0.2

GaO2[-]

-0.8 1

Ga (LLNL/GWB)

Ga (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 50: Eh-pH diagrams of the system Ga-O-H.

107

Ga = 10−10 , 298.15K, 105 Pa.

Table 31: List of Gd species FACT Gd[3+], Gd(s), Gd(s2), Gd2O3(s)

SUPCRT

LLNL

Gd[3+], Gd[4+], Gd[2+], GdOH[2+], GdO[+], GdO2H(aq), GdO2[-]

108

JNC-TDB

Gd (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Gd (FACT/FACTSAGE) 1.2

Gd2O3(s)

Gd[3+]

GdOH[2+] Gd[3+] GdO[+]

0.2

0.0

-0.2

-0.4

-0.6

GdO2H(aq) GdO2[-]

-0.8

-0.8 1

1.2

1.0

0.8

0.6

0.4

0.2

Gd (JNC-TDB/GWB)

1.2

Eh(V)

Gd (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 51: Eh-pH diagrams of the system Gd-O-H.

109

Gd = 10−10 , 298.15K, 105 Pa.

Table 32: List of Ge species FACT

SUPCRT

LLNL

HGeO3[-], Ge(s), GeO(s), GeO(s2), GeO2(s), GeO2(s2)

110

JNC-TDB

Ge (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Ge (FACT/FACTSAGE) 1.2

HGeO3[-]

0.2

0.0

-0.2

-0.4

-0.6

Ge(s)

-0.8

-0.8 1

Ge (LLNL/GWB)

Ge (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 52: Eh-pH diagrams of the system Ge-O-H.

111

Ge = 10−10 , 298.15K, 105 Pa.

Table 33: List of Hf species FACT Hf(s), Hf(s2), HfO2(s), HfO2(s2)

SUPCRT

LLNL

Hf[4+], HfOH[3+], HfO[2+], HHfO2[+], HfO2(aq), HHfO3[-]

112

JNC-TDB

Hf (FACT/FACTSAGE)

Hf (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

Hf[4+] HfOH[+3] HfO[2+]

0.4

Eh(V)

0.4 NO AQUEOUS SPECIES DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

HfO2(aq) HHfO3[-]

-0.8 1

Hf (LLNL/GWB)

Hf (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

HHfO2[-]

NO DATA

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 53: Eh-pH diagrams of the system Hf-O-H.

113

Hf = 10−10 , 298.15K, 105 Pa.

114

Table 34: List of Hg species FACT Hg[2+], Hg2[2+], HgOH[+], HHgO2[-], Hg(OH)2, Hg(aq), HgO(s)

SUPCRT Hg[2+], Hg2[2+], HgOH[+], HHgO2[-], HgO(aq), Hg(Quicksilver)

LLNL Hg[2+], Hg2[2+], Quicksilver

HATCHES Hg[2+], Hg(OH)2(aq), Hg(OH)3[-], Hg2OH[3+], Hg3(OH)3[3+], HgOH[+], HgO, Quicksilver

115

JNC-TDB

Hg (FACT/FACTSAGE)

Hg (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 Hg[2+]

Hg[2+] 0.8

0.8

0.6

0.6 Hg(OH)2(aq)

HgO(aq)

0.4

Eh(V)

0.4

Hg2[2+]

0.2

0.2 Hg(s)

0.0

Hg(aq)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Hg (LLNL/GWB)

Hg (JNC-TDB/GWB)

1.2

1.0

1.0 Hg[2+]

0.8

0.6

0.6 Hg2[2+] 0.4

Eh(V)

0.4

0.2

0.0

0.2

NO DATA

0.0 Quicksilver

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 54: Eh-pH diagrams of the system Hg-O-H (1).

116

Hg = 10−10 , 298.15K, 105 Pa.

1.2

Hg (HATCHES/FLASK-AQ)

1.0

0.8

Hg[2+]

0.6 Hg(OH)2(aq)

Eh(V)

0.4

0.2

Quicksilver

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 55: Eh-pH diagrams of the system Hg-O-H (2).

117

Hg = 10−10 , 298.15K, 105 Pa.

Table 35: List of Ho species FACT Ho[3+], Ho(s) , Ho(s2), Ho2O3(s), Ho2O3(s2)

SUPCRT

LLNL

Ho[3+], Ho[4+], Ho[2+], HoOH[2+], HoO[+], HoO2H(aq), HoO2[-]

118

JNC-TDB

Ho (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.4

Ho[3+]

Eh(V)

Ho (SUPCRT/FLASK-AQ)

1.2

0.2

Ho[3+] HoOH[2+]

0.2

HoO[+]

Ho2O3(s) 0.0

HoO2H(aq)

0.0

Ho2[-] -0.2

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ho (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Ho (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 56: Eh-pH diagrams of the system Ho-O-H.

119

Ho = 10−10 , 298.15K, 105 Pa.

120

Table 36: List of I species FACT

SUPCRT

LLNL

I[-], I3[-], IO[-], I[-], I3[-], IO[-], I[-] IO3[-], HIO(aq), IO3[-], HIO(aq), HIO3(aq), I2 (aq), HIO3(aq), IO4[-] H2OI[+], I2OH[-], I2(s)

JNC-TDB I[-], IO3[-], HIO3(aq), I3[-], IO[-], IO4[-], I2O[2-], HIO(aq), I2OH[-],I2(aq), HI(aq), H2OI[-], I2(s), I2(c), I(g), I2(g), HI(g)

HATCHES I[-], IO3[-], H2IO[+], HI(aq), HIO(aq), HIO3(aq), I2(aq), I2O[2-], I2OH[-], I3[-], IO[-], IO4[-], I2 Remarks JNC-TDB: I2(s) is originally given as I2 in the database file, but its detailed description is not given. Then (s) is appended to I2 to avoid confusion with I2(c).

121

I (FACT/FACTSAGE) 1.2

1.0

I (SUPCRT/FLASK-AQ) 1.2

HIO3(aq)

H2OI[+]

1.0

I2OH[-]

IO3[-]

0.6

0.4

0.4 I[-]

0.2

IO3[-]

0.8

Eh(V)

0.8

IO4[-]

HIO(aq)

0.0

-0.2

-0.4

-0.6

-0.8

I[-]

0.2

-0.8 1

I (LLNL/GWB)

I (JNC-TDB/GWB)

1.2

1.0

HIO3(aq) HIO(aq) IO4[-]

0.8

0.6

0.4

Eh(V)

I2(aq)

I[-]

0.2

IO3[-]

I[-]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

I2OH[-]

-0.8 1

Figure 57: Eh-pH diagrams of the system I-O-H (1).

122

I = 10−10 , 298.15K, 105 Pa.

1.2

1.0

I (HATCHES/FLASK-AQ) HIO3(aq) HIO(aq) H2IO[+]

IO4[-]

I2OH[-] 0.8 IO3[-]

0.6

Eh(V)

0.4

0.2 I[-]

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 58: Eh-pH diagrams of the system I-O-H (2).

123

I = 10−10 , 298.15K, 105 Pa.

Table 37: List of In species FACT In[3+], InOH[2+], In(OH)2[+], In[+], In[2+], In(s), In2O3(s), In2O3(s2)

SUPCRT

LLNL

In[3+], InOH[2+], InO[+], HInO2(aq), InO2[-]

124

JNC-TDB

In (FACT/FACTSAGE)

In (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.6 In[3+] 0.4

Eh(V)

0.4 InOH[2+] 0.2

InO[+] 0.2 HInO2(aq)

In2O3(s)

In(OH)2[+] 0.0

0.0

-0.2

-0.4

-0.4 In[+]

-0.6

-0.8 5

In (LLNL/GWB)

In (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

InO2[-]

-0.6

In(s)

-0.8

In[3+]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 59: Eh-pH diagrams of the system In-O-H.

125

In = 10−10 , 298.15K, 105 Pa.

126

Table 38: List of K species FACT K[+], K(s), KH(s), KO2(s), K2O(s), K2O2(s), KOH(s), KOH(s2)

SUPCRT K[+], KOH(aq), K2O (Potassium-oxide)

LLNL K[+], KOH(aq)

HATCHES K[+], KOH

127

JNC-TDB K[+], K(c), K(g)

K (FACT/FACTSAGE)

K (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

KO2(s) 1.0

K[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

K (LLNL/GWB)

K (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

K[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

K[+]

-0.8 1

Figure 60: Eh-pH diagrams of the system K-O-H (1).

128

K = 10−10 , 298.15K, 105 Pa.

1.2

K (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 K[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 61: Eh-pH diagrams of the system K-O-H (2).

129

K = 10−10 , 298.15K, 105 Pa.

130

Table 39: List of La species FACT La[3+], La(s), La(s2), La(s3), LaH2(s), La2O3(s)

SUPCRT

LLNL

La[3+], La[2+], LaOH[2+], LaO[+], LaO2H(aq), LaO2[-]

HATCHES La[3+], La2OH[5+], La5(OH)9[6+], LaOH[2+], La(OH)3

131

JNC-TDB

La (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

La (FACT/FACTSAGE) 1.2

La[3+]

0.2

0.0

La[3+]

0.2

LaOH[2+]

0.0 LaO[+]

-0.2

-0.4

-0.6

LaO2H(aq)

-0.8

-0.8 1

La (LLNL/GWB)

La (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

LaO2[-]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 62: Eh-pH diagrams of the system La-O-H (1).

132

La = 10−10 , 298.15K, 105 Pa.

La (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4 La[3+] 0.2 LaOH[2+] 0.0 La(OH)3(s) -0.2

-0.4

-0.6

-0.8 1

Figure 63: Eh-pH diagrams of the system La-O-H (2).

133

La = 10−10 , 298.15K, 105 Pa.

134

Table 40: List of Li species FACT Li[+], LiOH(aq), Li(s), LiH(s), Li2O(s), Li2O2(s), LiOH(s)

SUPCRT Li[+], LiOH(aq)

LLNL Li[+], LiOH(aq)

HATCHES Li[+]

135

JNC-TDB Li[+]

Li (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.4 Li[+]

0.2

Eh(V)

Li (FACT/FACTSAGE) 1.2

LiOH(aq)

Li[+] 0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Li (LLNL/GWB)

Li (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

LiOH(aq)

Li[+]

0.0

0.2 Li[+] 0.0

LiOH(aq)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 64: Eh-pH diagrams of the system Li-O-H (1).

136

Li = 10−10 , 298.15K, 105 Pa.

Li (HACHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4

0.2

Li[+]

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 65: Eh-pH diagrams of the system Li-O-H (2).

137

Li = 10−10 , 298.15K, 105 Pa.

Table 41: List of Lu species FACT Lu[3+], Lu(s), Lu2O3(s)

SUPCRT

LLNL

Lu[3+], Lu[4+], LuOH[2+], LuO[+], LuO2H(aq), LuO2[-]

138

JNC-TDB

Lu (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Lu (FACT/FACTSAGE) 1.2

Lu2O3(s)

Lu[3+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

LuOH[2+] LuO[+] LuO2[-]

-0.8 1

Lu (LLNL/GWB)

Lu (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Lu[3+]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 66: Eh-pH diagrams of the system Lu-O-H.

139

Lu = 10−10 , 298.15K, 105 Pa.

140

Table 42: List of Mg species FACT Mg[2+], MgOH[+], Mg(s), MgH2(s), MgO(s), Mg(OH)2(s)

SUPCRT Mg[2+], MgOH[+], MgO(Periclase), Mg(OH)2(Brucite)

LLNL Mg[2+], Mg2OH[3+], Mg4(OH)4[4+], MgOH[+], Brucite

HATCHES Mg[2+], MgOH[+], Mg(OH)2

141

JNC-TDB Mg[2+], MgOH[+], Periclase

Mg (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.4 Mg[2+]

0.2

Eh(V)

Mg (FACT/FACTSAGE) 1.2

MgOH[+]

0.0

Mg[2+]

0.2

0.0 MgOH[+]

-0.2

-0.4

-0.6

-0.8

-0.8 1

Mg (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Mg[2+]

MgOH[+]

Eh(V)

Mg (LLNL/GWB)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Mg[2+]

MgOH[+]

-0.8 1

Figure 67: Eh-pH diagrams of the system Mg-O-H (1).

142

Mg = 10−10 , 298.15K, 105 Pa.

Mg (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4 Mg[2+]

0.2

0.0 MgOH[+]

-0.2

-0.4

-0.6

-0.8 1

Figure 68: Eh-pH diagrams of the system Mg-O-H (2).

143

Mg = 10−10 , 298.15K, 105 Pa.

144

Table 43: List of Mn species FACT Mn[2+], Mn[3+], MnO4[2-], MnO4[-], MnOH[+], Mn(OH)3[], Mn(s), Mn(s2), Mn(s3), Mn(s4), MnO2(s), Mn2O3(s), Mn3O4(s), Mn3O4(s2), MnO(s)

SUPCRT Mn[2+], Mn[3+], MnO4[2-], MnO4[-], MnOH[+], HMnO2[-], MnO(aq), MnO2[2-], MnO(Manganosite)

LLNL Mn[2+], MnO4[-], MnO4[2-], Mn(OH)2(aq), Mn(OH)3[-], Mn(OH)4[2-], Mn2(OH)3[+], Mn2OH[3+], MnOH[+], Birnessite, Bixbyite, Hausmannite, Manganite, Manganosite, Mn(OH)2(am), Mn(OH)3(c), Pyrolusite, Todorokite

HATCHES Mn[2+], Mn[3+], MnO4[2-], Mn(OH)2(aq), Mn(OH)3[-], Mn(OH)4[2-], Mn2(OH)3[+], Mn2OH[3+], MnO4[-], MnOH[+], MnOH[2+], Birnessite, Bixbyite, Hausmannite, Manganite, Manganosite, Mn(OH)2, Mn(OH)3, Mn(OH)3(c), Mn3O4, MnOOH, Pyrolusite, Todorokite

145

JNC-TDB Mn[2+], Mn[3+], MnO4[2-], MnO4[-], MnOH[+], Mn(OH)3[-], Birnesite, Manganite, Pyrolusite

Mn (FACT/FACTSAGE)

Mn (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 MnO4[-]

MnO4[-] 0.8

0.8

0.6

0.6 MnO2(s)

MnO4[2-]

0.4 Mn2O3(s)

Mn[2+]

0.2

Eh(V)

0.4

Mn3O4(s) 0.0

Mn[2+]

0.2

MnOH[+] MnO(aq)

0.0

HMnO2[-] -0.2

-0.2

MnOH[+]

MnO2[2-] -0.4

-0.4 Mn(OH)3[-]

-0.6

-0.8

-0.8 1

Mn (LLNL/GWB)

Mn (JNC-TDB/GWB)

1.2

1.0

1.0 MnO4[-]

MnO4[-] 0.8

0.8

0.6

Pyrolusite

0.6

Pyrolusite MnO4[2-]

MnO4[2-]

0.4 Bixbyite

Mn[2+]

0.2

Eh(V)

0.4

Hausmannite 0.0

Mn[2+]

0.2

Manganite 0.0

MnOH[+]

-0.2

-0.2 MnOH[+]

Mn(OH)2(aq)

-0.4

Mn(OH)3[-]

-0.6

-0.8

MnOH3[-]

-0.6

-0.8 1

Figure 69: Eh-pH diagrams of the system Mn-O-H (1).

146

Mn = 10−10 , 298.15K, 105 Pa.

1.2

Mn (HATCHES/FLASK-AQ)

1.0 MnO4[-] 0.8

0.6 MnO4[2-] Pyrolusite

Eh(V)

0.4 Mn[2+]

Bixbyite

0.2

Mn3O4(s) 0.0

MnOH[+] Mn(OH)2(aq)

-0.2

Mn(OH)3[-] -0.4 Mn(OH)4[2-] -0.6

-0.8 1

Figure 70: Eh-pH diagrams of the system Mn-O-H (2).

147

Mn = 10−10 , 298.15K, 105 Pa.

148

Table 44: List of Mo species FACT MoO4[2-], Mo(s), MoO2(s), MoO3(s)

SUPCRT

LLNL

MoO4[2-], HMoO4[-]

HATCHES MoO4[2-], Mo[3+], MoO2[+], H2MoO4(aq), HMoO4[-], Mo7O21(OH)3[3-], Mo7O22(OH)2[4-], Mo7O23OH[5-], Mo7O24[6-], MoO[3+], MoO2[2+], MoO2OH[+], H2MoO4, Mo, MoO2, MoO3

149

JNC-TDB

Mo (FACT/FACTSAGE)

Mo (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

Eh(V)

MoO3(s)

MoO4[2-]

0.2

0.0

MoO4[2-]

0.0 MoO2(s)

-0.2

-0.4

-0.4 Mo(s)

-0.6

-0.8

-0.8 1

Mo (LLNL/GWB)

Mo (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

HMoO4[-]

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 71: Eh-pH diagrams of the system Mo-O-H (1).

150

Mo = 10−10 , 298.15K, 105 Pa.

1.2

Mo (HATCHES/FLASK-AQ) MoO2OH[+]

1.0

H2MoO4(aq)

0.8

0.6

Eh(V)

0.4 MoO2[+]

0.2 MoO4[2-]

0.0

-0.2 Mo[3+] -0.4

-0.6

MoO2(s)

Mo(s)

-0.8 1

Figure 72: Eh-pH diagrams of the system Mo-O-H (2).

151

Mo = 10â&#x2C6;&#x2019;10 , 298.15K, 105 Pa.

152

Table 45: List of N species FACT N2(aq), NH3(aq), NH4[+], N2H5[+], ONO[-], N2O2[2-], NO3[-], HONO(aq), N3[-], N2H4(aq), HN3(aq), NH4N3(s), N2O4(s), N2O5(s), NH4NO3(s)

SUPCRT N2(aq), NH3(aq), NH4[+], N2H5[+], NO2[-], N2O2[2-], NO3[-], HNO2(aq), HNO3(aq), H2N2O2(aq), HN2O2[-], N2H6[2+]

LLNL NO3[-], N2(aq), NH4[+], NO2[-], HNO2(aq), NH3(aq), N2(g)

HATCHES NO3[-], N2(aq), NH4[+], NO2[-], HNO3(aq), NH3(aq), NH4NO3(aq), NH4OH(aq)

153

JNC-TDB NO3[-], NH3(aq), NH4[+], NO2[-], N2(aq), N(g), N2(g), NH3(g)

N (FACT/FACTSAGE)

N (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 NO3[-]

0.8

0.6

0.4

Eh(V)

0.8

0.2 N2(aq)

0.0

NO3[-] N2(aq)

0.2

0.0

NH4[+]

NH4[+] -0.2

-0.2

-0.4

-0.4 NH3(aq)

-0.6

-0.8

-0.8 1

N (LLNL/GWB)

N (JNC-TDB/GWB)

1.2

1.0

1.0 NO3[-]

0.8

0.6

0.4

0.4 N2(aq)

0.2

NO3[-]

0.8

Eh(V)

NH3(aq)

-0.6

0.0

N2(aq)

0.2

0.0 NH4[+]

NH4[+]

-0.2

-0.4

-0.4 NH3

-0.6

NH3(aq)

-0.6

-0.8

-0.8 1

Figure 73: Eh-pH diagrams of the system N-O-H (1).

154

N = 10−10 , 298.15K, 105 Pa.

1.2

N (HATCHES/FLASK-AQ)

1.0 NO3[-]

0.8

0.6

Eh(V)

0.4

0.2

N2(aq)

0.0 NH4[+] -0.2

-0.4 NH4OH(aq)

-0.6

-0.8 1

Figure 74: Eh-pH diagrams of the system N-O-H (2).

155

N = 10−10 , 298.15K, 105 Pa.

156

Table 46: List of Na species FACT Na[+], Na(s), NaH(s), NaO2(s), Na2O(s2), Na2O(s3), Na2O2(s), Na2O2(s2), NaOH(s), NaOH(s2), Na2O(s)

SUPCRT Na[+], NaOH(aq), Na2O(Sodium-oxide)

LLNL Na[+], NaOH(aq)

HATCHES Na[+]

157

JNC-TDB Na+, Na(c), Na(g)

Na (FACT/FACTSAGE)

Na (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

Eh(V)

NaO2(s)

Na[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Na (LLNL/GWB)

Na (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Na[+]

0.2

Na[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Na[+]

0.2

-0.8 1

Figure 75: Eh-pH diagrams of the system Na-O-H (1).

158

Na = 10−10 , 298.15K, 105 Pa.

1.2

Na (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4

Na[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 76: Eh-pH diagrams of the system Na-O-H (2).

159

Na = 10â&#x2C6;&#x2019;10 , 298.15K, 105 Pa.

160

Table 47: List of Nb species FACT NbO3[-], Nb(OH)5(aq), Nb(OH)4[+], Nb(s), NbO(s), NbO2(s), NbO2(s2), NbO2(s3), Nb2O5(s)

SUPCRT

LLNL

NbO3[-], HNbO3(aq)

JNC-TDB Nb(OH)5(aq), Nb(OH)6[-], Nb2O5(s)

HATCHES Nb(OH)5(aq), Nb(OH)4[+], Nb(OH)6[-], Nb2O5(act)

161

Nb (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Nb(OH)5(aq)

Eh(V)

Nb (FACT/FACTSAGE) 1.2

NbO3[-]

0.2

0.0

-0.2

-0.4

-0.6

HNbO3(aq)

NbO3[-]

-0.6

NbO2(s) NbO(s)

-0.8

-0.8 1

Nb (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Nb (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Nb(OH)5(aq)

Nb(OH)6[-]

-0.8 1

Figure 77: Eh-pH diagrams of the system Nb-O-H (1).

162

Nb = 10−10 , 298.15K, 105 Pa.

1.2

Nb (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 Nb(OH)5(aq) 0.2

0.0

Nb(OH)6[-]

-0.2

-0.4

-0.6

-0.8 1

Figure 78: Eh-pH diagrams of the system Nb-O-H (2).

163

Nb = 10−10 , 298.15K, 105 Pa.

164

Table 48: List of Nd species FACT Nd[3+], Nd(s), Nd(s2), NdH2(s), Nd2O3(s), Nd2O3(s2)

SUPCRT

LLNL

JNC-TDB Nd[3+]

Nd[3+], Nd[4+], Nd[2+], NdOH[2+], NdO[+], NdO2H(aq), NdO2[-]

HATCHES Nd[3+], Nd(OH)2[+], Nd(OH)3(aq), NdOH[2+], Nd(OH)3

165

Nd (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.6 Nd[3+]

0.2

Nd2O3(s)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NdOH[2+]

NdO[+] NdO2H(aq) NdO2[-]

-0.8 1

Nd (LLNL/GWB)

Nd (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Nd[3+]

0.4

Eh(V)

0.4

Eh(V)

Nd (SUPCRT/FLASK-AQ)

1.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Nd[3+]

0.2

-0.8 1

Figure 79: Eh-pH diagrams of the system Nd-O-H (1).

166

Nd = 10−10 , 298.15K, 105 Pa.

Nd (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6 Nd[3+]

Eh(V)

0.4

0.2

Nd(OH)2[+]

0.0

Nd(OH)3(aq)

-0.2

-0.4

-0.6

-0.8 1

Figure 80: Eh-pH diagrams of the system Nd-O-H (2).

167

Nd = 10−10 , 298.15K, 105 Pa.

168

Table 49: List of Ni species FACT Ni[2+], NiOH[+], HNiO2[-], Ni2H(s), NiOOH(s), Ni(OH)2(s), NiO2(H2O)(s), Ni(s), NiO(s)

SUPCRT Ni[2+], NiOH[+], HNiO2[-], NiO(aq), NiO2[2-], Ni(Nickel), NiO(Bunsenite)

LLNL Ni[2+], Ni(OH)2, Ni(OH)3[-], Ni(OH)4[2-], Ni2OH[3+], Ni4(OH)4[4+], NiOH[+], Ni(OH)2(s), NiO(s)

HATCHES Ni[2+], Ni(OH)[+], Ni(OH)2(aq), Ni(OH)3[-], Ni2(OH)[3+], Ni4(OH)4[4+], Ni(OH)2, NiO

169

JNC-TDB Ni[2+], Ni(OH)2(aq), Ni(OH)3[-], NiOH[+], Ni2(OH)[+], Ni4(OH)[+], Ni(OH)2(s), NiO(c)

Ni (FACT/FACTSAGE)

Ni (SUPCRT/FLASK-AQ)

1.2

1.2 NiO2(H2O)(s)

1.0

NiOOH(s) 0.8

0.8

0.6

0.6 NiOH[+] HNiO2[-]

Ni[2+]

0.2

0.4

Eh(V)

0.4

Ni[2+]

0.2

0.0

-0.2

-0.4

HNiO2[-] NiO2[2-]

-0.6

-0.6 Ni(s)

Ni2H(s)

Ni(s)

-0.8

-0.8 1

1.2

1.0

0.8

0.6

0.4

0.4 Ni[2+]

0.2

Ni (JNC-TDB/GWB)

1.2

Eh(V)

Ni (LLNL/GWB)

NiOH[+] Ni(OH)2(aq)

0.0

Ni[2+]

0.2

Ni(OH)3[-] Ni(OH)2(aq)

0.0

Ni(OH)3[-] Ni(OH)4[2-]

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 81: Eh-pH diagrams of the system Ni-O-H (1).

170

Ni = 10−10 , 298.15K, 105 Pa.

Ni (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4

Ni[2+]

0.2 Ni(OH)[+] 0.0

Ni(OH)2(aq)

-0.2

Ni(OH)3[-]

-0.4

-0.6

-0.8 1

Figure 82: Eh-pH diagrams of the system Ni-O-H (2).

171

Ni = 10−10 , 298.15K, 105 Pa.

172

Table 50: List of Np species FACT

SUPCRT

LLNL

JNC-TDB

Np[4+], Np[3+], NpO Np[4+], Np[3+], NpO [+], NpO 2[+] NpO2 OH(am), NpO2(OH)2[-] 2[2+], (NpO 2)2(OH)2 [2+], (NpO2)3(OH)5 NpO2[2+], N [+], Np(OH)2[2+], pOH[3+], N Np(OH)3[+], Np(OH)4 p(OH)4(s), NpO2(am), (aq), Np(O NpO2OH(am) H)5[-], NpO2OH(aq), NpO2OH[+], NpOH[2+], NpOH[3+], Np(s), Np(OH)4(s), Np2O5(s), NpO2(s), N pO2(OH)(am), NpO2(O H)2(s)

Np(s), NpO2(s), NpO 3(H 2O)(s)

HATCHES

OECD-NEA

OECD-NEA update

Np[4+], Np[3+], NpO 2[+], NpO 2[2+], Np (OH)2[+], Np(OH)3(a q), Np(OH)4(aq), Np (OH)4[-], Np2(OH)2[4 +], NpO22OH2[2+], Np O23OH5[+], NpO2OH(a q), NpO2OH[+], NpO2 OH2[-], NpOH[2+], N pOH[3+], Np, Np(OH) 3, Np(OH) 4, Np 2O5, N pO2, NpO2(am), NpO2 (OH)2, NpO2OH, NpO2O H(am,aged), NpO2OH (am,fresH), NpO3*H2 O(cr)

Np[4+], Np[3+], NpO 2[+], NpO 2[2+], NpO H[2+], NpOH[3+], N pO2OH(aq), NpO2OH [+], NpO2(OH)2[-], Np(OH)4(aq), (NpO2)2 (OH)2[2+], (NpO2)3(O H)5[+], Np(c), NpO2 (am_hyd), NpO2(c), Np2O5(c), NpO2OH(am_ aged), NpO2OH(am_fr esh), NpO2(OH)2(c), NpO3H2O(c)

Np[4+], Np[3+], NpO 2[+], NpO 2[2+], NpO H[2+], NpOH[3+], N p(OH)2[2+], NpO2OH (aq), NpO2OH[+], Np O2(OH)2[-], Np(OH)4 (aq), (NpO2)2(OH)2[2 +], (NpO2)3(OH)5[+], Np(cr), NpO2(cr), N p2O5(cr), NpO2(OH)2 (cr), NpO3H2O(cr)

173

Np (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Np (FACT/FACTSAGE) 1.2

NO AQUEOUS SPECIES DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Np (LLNL/GWB)

1.2

NpO2OH[+] (NpO2)3(OH)5[+] NpO2(OH)2(s)

1.0

NpO2[+]

0.8

Np (JNC-TDB/GWB)

1.2

0.8 NpO2OH(aq)

0.6

NpO2[+]

0.6

0.4

NpO2OH(aq)

0.4 Np[4+]

Eh(V)

NO DATA

0.2

0.0

Np[4+] 0.2

NpOH[3+] NpO2OH2[-]

0.0 NpO2(s)

-0.2

-0.2 Np(OH)5[-]

-0.4

-0.6

NP(OH)4(aq)

Np[3+]

Np[3+] -0.6

-0.8

-0.8 1

Figure 83: Eh-pH diagrams of the system Np-O-H (1).

174

Np = 10−10 , 298.15K, 105 Pa.

Np (OECD-NEA/FLASK-AQ) 1.2

Np (HATCHES/FLASK-AQ) NpO2[2+]

1.2

1.0

Np[4+]

NpO2[+] NpO2OH(aq) NpO2(OH)2[-]

0.6

NpO2[+]

0.4

NpO2OH(aq) NpOH[3+]

NpO2OH2[-]

0.2 Np[3+]

Eh(V)

NpO2(OH)2(c)

0.8

0.4

0.0

NpO2OH[+]

1.0

NpO2(OH)2(s)

0.8

0.6

NpO2[2+]

NpO2OH[+]

Np[4+]

NpO2(c)

0.2

0.0

-0.2

NpO2(s)

Np[3+] -0.4

-0.4

-0.6

-0.8

-0.8 1

Np (OECD-NEA update/FLASK-AQ) 1.2 NpO2OH[+]

NpO2[2+] 1.0

NpO2(OH)2(cr)

0.8

NpO2[+]

0.6

Eh(V)

0.4

NpO2OH(aq)

NpOH[3+]

NpO2(OH)[-]

Np(OH)2[2+] 0.2 NpO2(cr)

0.0

-0.2

-0.4

Np[3+]

-0.6

-0.8 1

Figure 84: Eh-pH diagrams of the system Np-O-H (2).

175

Np = 10−10 , 298.15K, 105 Pa.

Table 51: List of Os species FACT

SUPCRT

LLNL

OsO4(aq), HOsO5[-], H2OsO5[-], Os(s), OsO2(s), OsO4(s), OsO4(s2), Os(OH)4(s)

176

JNC-TDB

Os (FACT/FACTSAGE)

Os (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.8 OsO4(aq)

0.6

0.4 HOsO5[-]

0.2

OsO2(s)

Eh(V)

0.4

0.0

NO DATA

0.2

0.0 Os(s)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Os (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Os (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 85: Eh-pH diagrams of the system Os-O-H.

177

Os = 10−10 , 298.15K, 105 Pa.

178

Table 52: List of P species FACT

SUPCRT

LLNL

PO4[3-], P2O7[4-], HPO3[2-], H2PO3[-], HPO4[2-], H2PO4[-], H3PO4(aq), HP2O7[3], H2P2O7[2-], H3P2O7[-], H4P2O7(aq), PH3(aq), PH4[+], P(s), P(s2), P(s3), P(s4), (P2O5)2(s), H3PO4(s), (H3PO4)2(H2O)(s)

PO4[3-], P2O7[4-], HPO3[2-], HPO4[2-], H2PO4[-], H3PO4(aq), HP2O7[3-], H3P2O7[-], H4P2O7(aq),H3PO2(aq), H2PO2[-], H3PO3(aq), H2P2O7[2-], H2PO3[-]

HPO4[2-], H2P2O7[2-], H2PO4[-], H3P2O7[-] H3PO4(aq), H4P2O7(aq), HP2O7[3-], P2O7[4-], PO4[3-]

HATCHES PO4[3-], H2PO4[-], HPO4[2-], H2P2O7[2], H3P2O7[-], H3PO4(aq), H4P2O7(aq), HP2O7[3], P2O7[3-]

179

JNC-TDB PO4[3-], P2O7[4-], HPO4[2-], H2PO4[-], H3PO4(aq), HP2O7[3], H2P2O7[2-], H3P2O7[-], H4P2O7(am), P(am) P(c), P(g), P2(g), P4(g)

P (FACT/FACTSAGE)

P (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.6 H3PO4(aq) H4P2O7(aq)

0.4

0.2

Eh(V)

0.4

H2PO4[-]

HPO4[2-]

0.2

HPO4[2-]

PO4[3-]

0.0

-0.2

-0.2 H2PO3[-]

-0.4

-0.6

-0.4

PO4[3-]

H3PO3(aq) H2PO3[-]

-0.6

PH3(aq)

H3PO2(aq)

HPO3[2-] -0.8 1

P (LLNL/GWB)

HPO3[2-]

H2PO2[-]

-0.8

P (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.6 H3PO4(aq) 0.4 H2PO4[-]

Eh(V)

0.4 HPO4[2-]

0.2

0.2 H3PO4(aq)

H2PO4[-]

HPO4[2-]

PO4[3-]

PO4[3-] 0.0

0.0

-0.2

-0.4

-0.6

-0.8

P(s) 1

Figure 86: Eh-pH diagrams of the system P-O-H (1).

180

P = 10−10 , 298.15K, 105 Pa.

P (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6 H3PO4(aq) 0.4

Eh(V)

H2PO4[-]

0.2

HPO4[2-] PO4[3-]

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 87: Eh-pH diagrams of the system P-O-H (2).

181

P = 10−10 , 298.15K, 105 Pa.

182

Table 53: List of Pa species FACT

SUPCRT

LLNL

JNC-TDB Pa[4+], PaO(OH)3(aq) PaO(OH)2(aq), PaOOH[2+], Pa(OH)[3+], Pa(OH)2[+], Pa(OH)3[+], PaO2(s), Pa2O5(s)

HATCHES Pa[4+], PaO2[+], Pa(OH)[3+], Pa(OH)2[2+], Pa(OH)3[+], Pa(OH)4(aq), PaO(OH)[2+], PaO2(OH)(aq), Pa2O5, PaO2

183

Pa (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Pa (FACT/FACTSAGE) 1.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Pa (LLNL/GWB)

Pa (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.6 PaOOH[2+] PaO(OH)2(aq)

0.4

Eh(V)

0.4 NO DATA

0.2

PaO(OH)3(aq)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Pa(OH)[3+] Pa(OH)2[2+] Pa(OH)3[+]

Figure 88: Eh-pH diagrams of the system Pa-O-H (1).

184

Pa = 10−10 , 298.15K, 105 Pa.

Pa (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6 PaO2[+]

Eh(V)

0.4

0.2 PaO2(OH)(aq)

0.0

-0.2 Pa(OH)[3+] -0.4 Pa(OH)2[2+] -0.6

Pa(OH)4(aq)

-0.8 1

Figure 89: Eh-pH diagrams of the system Pa-O-H (2).

185

Pa = 10−10 , 298.15K, 105 Pa.

186

Table 54: List of Pb species FACT Pb[2+], PbOH[+], HPbO2[-], Pb3(OH)4[2+], Pb4(OH)4[4+], Pb6(OH)8[4+], Pb(s), PbO(s2), PbO2(s), Pb3O4(s), Pb(OH)2(s), (PbO)3(H2O)(s), PbO(s)

SUPCRT Pb[2+], PbOH[+], HPbO2[-], PbO(aq), PbO(Litharge)

LLNL Pb[2+]

HATCHES Pb[2+], Pb(iv)[4+], Pb(OH)[+], Pb(OH)2(aq), Pb(OH)3[+], Pb(OH)3[-], Pb(OH)4(aq), Pb2(OH)[3+], Pb3(OH)4[2+], Pb6(OH)8[4+], Pb, Pb(OH)2, Pb3O4, PbO, PbO2

187

JNC-TDB Pb[2+], PbOH[+], Pb(OH)2(aq), Pb(OH)3[-], Pb2(OH)[+], Pb4(OH)4[4+], Pb3(OH)4[2+], Pb3(OH)5[+] Pb6(OH)8[4+], Pb(c) PbO(red), PbO(yellow) Pb(OH)2(s), PbO2(s), Pb3O4(s)

Pb (FACT/FACTSAGE)

Pb (SUPCRT/FLASK-AQ)

1.2

1.0

PbO2(s)

0.8

0.6

0.4

Eh(V)

1.0

Pb[2+]

0.2

Pb[2+]

0.2

PbOH[+]

PbOH[+] 0.0

PbO(aq)

0.0 HPbO2[-]

HPbO2[-]

-0.2

-0.4

-0.4 Pb(s)

-0.6

-0.8

-0.8 1

Pb (LLNL/GWB)

Pb (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

PbO2(s)

Pb[2+]

0.2

Pb[2+]

0.2

PbOH[+]

0.0

-0.2

-0.4

-0.6

Pb(OH)2(aq) Pb(OH)3[-]

Pb(c) -0.8

-0.8 1

Figure 90: Eh-pH diagrams of the system Pb-O-H (1).

188

Pb = 10−10 , 298.15K, 105 Pa.

1.2

Pb (HATCHES/FLASK-AQ)

1.0 Pb(OH)4(aq)

0.8

0.6

0.4

Eh(V)

Pb[2+]

0.2 Pb(OH)[+] 0.0 Pb(OH)2(aq)

-0.2

Pb(OH)3[-]

-0.4

-0.6 Pb(s) -0.8 1

Figure 91: Eh-pH diagrams of the system Pb-O-H (2).

189

Pb = 10−10 , 298.15K, 105 Pa.

Table 55: List of Pd species FACT Pd[2+], PdO2(s), Pd(s), PdO(s)

SUPCRT

LLNL

JNC-TDB Pd[2+], Pd(c)

Pd[2+], PdOH[+], PdO(aq), Pd(Palladium), PdO(s), Pd(OH)2(s)

190

Pd (FACT/FACTSAGE)

Pd (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

Pd[2+] PdOH[+]

Pd[2+] PdO2(s)

0.6

PdO(s)

0.2

0.0

PdO(aq)

0.4

Eh(V)

0.4

Eh(V)

0.6

0.2

0.0

Pd(s)

-0.2

-0.4

-0.6

-0.8

Pd(s)

-0.8 1

Pd (LLNL/GWB)

Pd (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Pd[2+]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Pd(c)

-0.8 1

Figure 92: Eh-pH diagrams of the system Pd-O-H.

191

Pd = 10−10 , 298.15K, 105 Pa.

Table 56: List of Pm species FACT

SUPCRT

LLNL

Pm[4+], Pm[3+], Pm[2+]

192

JNC-TDB

1.2

Pm (FACT/FACTSAGE)

1.2

0.8

0.6

0.4

Eh(V)

1.0

Eh(V)

1.0

NO DATA

0.2

Pm (SUPCRT/FLASK-AQ)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Pm[3+]

-0.8 1

Pm (JNC-TDB/GWB)

Pm (LLNL/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 93: Eh-pH diagrams of the system Pm-O-H.

193

Pm = 10−10 , 298.15K, 105 Pa.

Table 57: List of Po species FACT

SUPCRT

LLNL

JNC-TDB Po[4+], Po(OH)4(s)

Po[2+], Po[4+], Po(OH)2[4+], Po(s)

194

Po (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Po (FACT/FACTSAGE) 1.2

Po(OH)2[4+]

0.2

0.0

-0.2

-0.2 Po(s)

-0.4

-0.6

-0.8

-0.8 1

Po (JNC-TDB/GWB)

Po (LLNL/GWB) 1.2

1.2

1.0

0.8

0.6

0.4

Eh(V)

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Po(OH)4(s)

Po[4+]

0.2

-0.8 1

Figure 94: Eh-pH diagrams of the system Po-O-H.

195

Po = 10−10 , 298.15K, 105 Pa.

Table 58: List of Pr species FACT Pr[3+], PrOH[2+], Pr(OH)2[+], Pr(s), Pr(s2), PrH2(s), PrO2(s), Pr2O3(s), Pr6O11(s), Pr7O12(s), PrO3H3(s)

SUPCRT

LLNL

Pr[3+], PrOH[2+], PrO[+], Pr[4+], Pr[2+], PrO2H(aq), PrO2[-]

196

JNC-TDB

Pr (FACT/FACTSAGE)

Pr (SUPCRT/FLASK-AQ)

1.2

1.0

PrO2(s)

0.8

0.6

0.4

0.4 Pr[3+]

0.2

Eh(V)

1.0

Pr(OH)2[+]

Pr[3+]

0.2

0.0

-0.2

-0.4

-0.6

PrOH[2+] PrO[+] PrO2H(aq)

-0.8

-0.8 1

Pr (LLNL/GWB)

Pr (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

PrO2[-]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 95: Eh-pH diagrams of the system Pr-O-H.

197

Pr = 10−10 , 298.15K, 105 Pa.

Table 59: List of Pt species FACT Pt[2+], Pt(s)

SUPCRT

LLNL

Pt[2+], PtOH[+], PtO(aq), Pt(Platinum)

198

JNC-TDB

Pt (FACT/FACTSAGE)

Pt (SUPCRT/FLASK-AQ)

1.2

1.0

Pt[2+]

0.8

0.6

0.4

Eh(V)

1.0

0.2

PtO(aq)

0.2 Pt(s)

Pt(s) 0.0

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Pt (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Pt (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 96: Eh-pH diagrams of the system Pt-O-H.

199

Pt = 10−10 , 298.15K, 105 Pa.

200

Table 60: List of Pu species FACT

SUPCRT

Pu[3+], Pu(s), Pu(s 2), Pu(s3), Pu(s4), Pu(s5), Pu(s6), PuH 2(s), PuH3(s), PuO 2 (s), Pu2O3(s), Pu5O8 (s)

HATCHES

OECD-NEA

Pu[4+], Pu[3+], PuO Pu[4+], Pu[3+], PuO 2[+], PuO 2[2+], Pu 2[+], PuO 2[2+], PuO (OH)[2+], Pu(OH)[3 H[2+], PuOH[3+], P +], Pu(OH)2[+], Pu uO2OH[+], PuO2(OH)2 (aq), (PuO2)2(OH)2[2 (OH)2[2+], Pu(OH)3 (aq), Pu(OH)3[+], P +], Pu(c), PuO1.61(c u(OH)4(aq), Pu(OH)4 _bcc), PuO2(c), PuO [-], Pu2(OH)2[4+], 2(hyd_aged), Pu 2O3 Pu2(OH)2[6+], Pu2(OH) (c), PuO2OH(am), Pu 3[5+], Pu 2(OH) 4[4+], (OH)3(c), PuO2(OH)2H Pu2(OH)5[3+], Pu3(OH) 2O(c) 5[4+], PuO 2(OH) 2[-], (PuO2)2OH2[2+], (PuO 2)3OH5[+], PuO 2OH(a q), PuO2OH[+], PuO2 OH2(aq), PuO2OH3[-], Pu(OH)3, Pu(OH)4, P u2O3, PuO2(OH)2*H2O (c), PuO2, PuO2(a), PuO2(OH)2, PuO2OH, P u(OH)3(c)

LLNL

JNC-TDB

PuO2[2+], Pu[3+], Pu[4+], PuO2[+], (PuO2)2(OH)2[2+], P (PuO2)3(OH)5[+], u(OH)2[2+], Pu(OH)3 [+], Pu(OH)4(aq), Pu(OH) PuO2OH 5[-], (aq), PuO2OH[+], PuOH[2+], PuOH[3+], Pu(OH)3(a q), Pu(OH)3(s), Pu(OH)4(am), Pu(OH) 4(s), Pu2O3(c,beta), PuO2(s), PuO2(OH)2 (s), PuO2(OH) 2(c), PuO 2(c), PuO2OH(am)

Pu[4+], Pu[3+], Pu OH[2+], PuOH2[+], P u(OH)3(aq), PuO2[+], PuO2OH(aq), PuO2(O H)2[-], PuO2[2+], P uO2OH[+], PuO2(OH)2, PuO2OH3[-], Pu(OH)4 (aq), PuOH[3+], Pu (OH)3(am), Pu(OH)3 (c), PuO2(am), PuO2 OH(s)

OECD-NEA update Pu[4+], Pu[3+], Pu O2[+], PuO2[2+], Pu OH[2+], PuOH[3+], Pu(OH)2[2+], Pu(OH) 3[+], PuO 2OH(aq), P uO2OH[+], PuO2(OH)2 (aq), Pu(OH)4(aq), (PuO2)2(OH)2[2+], Pu (cr), PuO1.61(bcc), PuO2(cr), Pu2O3(cr), Pu(OH)3(cr), PuO2(O H)2H2O(cr)

201

Pu (FACT/FACTSAGE)

Pu (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

0.2

Pu[3+]

Eh(V)

1.2

Eh(V)

1.2

0.2

PuO2(s)

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Pu (LLNL/GWB)

Pu (JNC-TDB/GWB)

1.2

1.0

NO DATA

1.2 Pu[4+]

PuO2[2+]

PuO2[2+] PuO2OH[+]

1.0

Pu[4+]

PuO2OH[+]

PuO2(OH)2(s) 0.8

PuO2(OH)2

0.8

PuO2(OH)3[-]

PuO2[+]

0.4

0.2

Pu[3+]

Eh(V)

0.6

Eh(V)

0.6

Pu[3+]

0.2

PuO2(s)

0.0

-0.2

-0.4

PuO2(am)

PuOH[2+] -0.6

-0.6

Pu(OH)2[+]

PuOH[2+] -0.8

Pu(OH)3(c)

-0.8 1

Figure 97: Eh-pH diagrams of the system Pu-O-H (1).

202

Pu = 10−10 , 298.15K, 105 Pa.

1.2

Pu (OECD-NEA/FLASK-AQ)

Pu (HATCHES/FLASK-AQ)

1.2

PuO2OH[+] 1.0

PuO2[2+]

1.0

PuO2(OH)2(aq)

PuO2[+]

PuO2(OH)3[-]

0.8

0.6

PuO2(OH)2(aq)

PuO2[+]

0.8

0.6

0.4 PuO2(OH)2[-]

PuO2(s)

Eh(V)

Pu[3+]

Eh(V)

0.4

PuO2OH[+]

PuO2[2+]

0.2

0.0

-0.2

-0.4

-0.6

Pu[3+] PuO2(c)

-0.6 PuOH[2+]

Pu(OH)[2+] -0.8

-0.8 1

Pu (OECD-NEA update/FLASK-AQ) 1.2 PuO2[2+] 1.0

PuO2OH[+]

Pu(OH)2[2+] PuO2(OH)2(aq)

PuO2[+]

0.8

0.6

Eh(V)

0.4

0.2 Pu[3+] PuO2(cr)

0.0

-0.2

-0.4

-0.6 PuOH[2+] -0.8 1

Figure 98: Eh-pH diagrams of the system Pu-O-H (2).

203

Pu = 10−10 , 298.15K, 105 Pa.

204

Table 61: List of Ra species FACT Ra[2+], Ra(s)

SUPCRT

LLNL

Ra[2+]

JNC-TDB Ra[2+], RaOH[+]

HATCHES Ra[2+], RaOH[+], Ra(c)

205

Ra (FACT/FACTSAGE)

Ra (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

Ra[2+]

0.2

Ra[2+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ra (LLNL/GWB)

Ra (JCN-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

Ra[2+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Ra[2+]

RaOH[+]

-0.8 1

Figure 99: Eh-pH diagrams of the system Ra-O-H (1).

206

Ra = 10−10 , 298.15K, 105 Pa.

Ra (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4 Ra[2+]

0.2

0.0 RaOH[+] -0.2

-0.4

-0.6

-0.8 1

Figure 100: Eh-pH diagrams of the system Ra-O-H (2).

207

Ra = 10−10 , 298.15K, 105 Pa.

Table 62: List of Rb species FACT Rb[+], Rb(s), Rb2O(s), RbOH(s)

SUPCRT Rb[+], RbOH(aq)

LLNL Rb[+]

208

JNC-TDB

Rb (FACT/FACTSAGE)

Rb (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

Rb[+]

0.2

Rb[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Rb (LLNL/GWB)

Rb (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

Rb[+]

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 101: Eh-pH diagrams of the system Rb-O-H.

209

Rb = 10−10 , 298.15K, 105 Pa.

Table 63: List of Re species FACT ReO4[-], Re[-], Re[+], Re(s), ReO2(s), ReO3(s), Re2O7(s), HReO4(s)

SUPCRT

LLNL

ReO4[-]

210

JNC-TDB

Re (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.6 ReO4[-]

0.4

Eh(V)

0.4

Eh(V)

Re (SUPCRT/FLASK-AQ)

1.2

0.2 Re[+]

0.0

ReO4[-]

0.2

0.0

-0.2

-0.4

-0.4 Re[-]

-0.6

-0.8

-0.8 1

Re (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Re (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 102: Eh-pH diagrams of the system Re-O-H.

211

Re = 10−10 , 298.15K, 105 Pa.

Table 64: List of Rh species FACT RhO(s), RhO2(s), Rh(s), Rh2O(s), Rh2O3(s)

SUPCRT

LLNL

Rh[3+], RhOH[+], RhOH[2+], Rh[2+], RhO(aq), RhO[+], Rh(Rhodium), Rh2O(s), Rh2O3(s)

212

JNC-TDB

Rh (FACT/FACTSAGE)

Rh (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

Eh(V)

Rh[3+]

NO AQUEOUS SPECIES DATA

0.2

Rh2O3(s) Rh[2+]

RhOH[+] RhO(aq)

0.0

-0.2

-0.4

-0.6

Rh(s)

-0.8 1

Rh (LLNL/GWB)

Rh (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

RhO[+]

0.2

0.0

-0.8

RhOH[2+]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 103: Eh-pH diagrams of the system Rh-O-H.

213

Rh = 10−10 , 298.15K, 105 Pa.

214

Table 65: List of Ru species FACT RuO4[2-], RuO4[-], RuO4(aq), Ru(OH)2[2+], RuO4(s), Ru(s), RuO2(s)

SUPCRT RuO4[2-], Ru[3+], Ru[2+], RuOH[+], RuOH[2+], RuO(aq), RuO[+], Ru(Ruthenium), RuO2(s)

LLNL Ru[3+], Ru(OH)2[2+], Ru[2+], RuO4(aq), RuO4[-], RuO4[2-], H2RuO5(aq), HRuO5[-], Ru(OH)2[+], Ru4(OH)12[4+], RuOH[2+], Ru(OH)3*H2O(am), Ru(c), RuO2(s), RuO2*2H2O(am), RuO4(s), Ru(g), RuO4(g)

HATCHES Ru[3+], Ru(OH)2[2+], Ru[2+], RuO4[-], RuO4[2-], H2RuO5(aq), HRuO5[], Ru(OH)[2+], Ru(OH)2[+], Ru4(OH)12[4+], Ru(c), Ru2O5, RuO2(s), RuO2*2H2O, RuO4(s), Ru(OH)3*H2O

215

JNC-TDB

Ru (FACT/FACTSAGE)

Ru (SUPCRT/FLASK-AQ)

1.2

1.2 RuO4(aq)

1.0

1.0 Ru(OH)2[2+]

RuO4[-]

0.8

0.6 RuO2(s)

Ru[3+]

0.2

0.0

RuO2(s) RuO[+]

0.4

Eh(V)

0.4

Eh(V)

RuO4[2-]

0.6 RuO4[2-]

0.2

0.0 Ru(s)

Ru(s)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Ru (LLNL/GWB)

Ru (JNC-TDB/GWB)

1.2

1.2 H2RuO5(aq)

HRuO5[-]

1.0

Ru(OH)2[2+] 0.8

0.8

RuO4[-]

0.6

0.6 Ru[3+] 0.4

Eh(V)

RuO4[2-]

RuO2(s)

Ru(OH)2[+]

0.4

0.2

0.0

NO DATA

0.2

0.0 Ru(s)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 104: Eh-pH diagrams of the system Ru-O-H (1).

216

Ru = 10−10 , 298.15K, 105 Pa.

Ru (HATCHES/FLASK-AQ) 1.2 H2RuO5(aq) 1.0

HRuO5[-]

Ru(OH)2[2+] RuO4[-]

0.8

0.6

RuO4[2-]

Ru[3+] RuO2(s)

Ru(OH)2[+]

Eh(V)

0.4

0.2

0.0 Ru(c) -0.2

-0.4

-0.6

-0.8 1

Figure 105: Eh-pH diagrams of the system Ru-O-H (2).

217

Ru = 10−10 , 298.15K, 105 Pa.

218

Table 66: List of S species FACT S[2-], S2[2-], S3[2-], S4[2-], S5[2-], HS[-], H2S(aq), SO2(aq), SO3[2-], SO4[2-], S2O3[2-], S2O4[2-], S2O5[2-], S2O6[2-], S2O8[2-], S3O6[2-], S4O6[2-], S5O6[2-], HSO3[-], HSO4[-], HS2O4[-], H2S2O4 (aq), S(s), S(s2), SO3(s)

SUPCRT

LLNL

SO4[2-], HS[-], S2[2-], S3[2-], S4[2-], S5[2-], H2S(aq), HS[-], H2S(aq), H2SO4(aq), HSO4[-], SO2(aq), SO3[2-], S[2-], S2[2-], SO4[2-], S2O3[2-], S3[2-], S4[2-], S2O4[2-], S2O5[2-], S5[2-], S6[2-], S2O6[2-], S2O8[2-], Sulfur(rhmb), S3O6[2-], S4O6[2-], H2S(g), S2(g) S5O6[2-], HSO3[-], HSO4[-], HS2O4[-], H2S2O4 (aq), HSO5[], HS2O3[-], H2S2O3(aq), S(Sulfur)

HATCHES SO4[2-], HS[-], S2[2-], S3[2-], S4[2-], S5[2-], SO2(aq), H2S(aq), H2S2O3(aq), H2S2O4(aq), H2SO3(aq), HS2O3[-], HS2O4[-], HSO3[-], HSO4[-], S[2-], S2O3[2-], S2O4[2-], S2O5[2-], S2O6[2-], S2O8[2-], S3O6[2-], S4O6[2-], S5O6[2-], SO3[2-], S(c), Sulfur-rhmb

219

JNC-TDB SO4[2-], S[2-], SO3[2-], S2O3[2-], HS[-], H2S(aq), HSO3[-], HS2O3[-], H2SO3(aq), HSO4[-], S(c), S(g), S2(g), SO2(g), H2S(g)

S (FACT/FACTSAGE)

S (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

HSO4[-]

0.4

0.2

Eh(V)

0.4

HSO4[-]

SO4[2-]

0.0

SO4[-]

0.2

0.0 H2S(aq)

H2S(aq)

-0.2

-0.4

-0.4 HS[-]

HS[-] -0.6

-0.6 S[2-]

-0.8

-0.8 1

S (LLNL/GWB)

S (JNC-TDB/GWB)

1.2

1.0

0.8

0.8 HSO4[-]

0.6

0.4

Eh(V)

SO4[2-]

0.2

HSO4[-]

0.2

0.0

-0.2

SO4[-]

H2S(aq)

-0.4

H2S(aq)

HS[-] -0.6

-0.6

HS[-] S[2-]

-0.8

-0.8 1

Figure 106: Eh-pH diagrams of the system S-O-H (1).

220

S = 10−10 , 298.15K, 105 Pa.

1.2

S (HATCHES/FLASK-AQ)

1.0

0.8

0.6

HSO4[-]

0.4

Eh(V)

SO4[2-]

0.2

0.0 H2S(aq) -0.2

-0.4 HS[-] -0.6 S[2-] -0.8 1

Figure 107: Eh-pH diagrams of the system S-O-H (2).

221

S = 10−10 , 298.15K, 105 Pa.

222

Table 67: List of Sb species FACT SbO2[-], HSbO2(aq), SbO[+], Sb(s), SbO2(s), Sb2O3(s), Sb2O3(s2), Sb2O4(s), Sb2O5(s)

SUPCRT

LLNL

SbO2[-], HSbO2(aq)

JNC-TDB Sb(OH)3(aq), Sb(OH)5(aq) Sb(OH)6[-], Sb12(OH)64(aq) Sb12(OH)65[5-], Sb12(OH)66[6-], Sb12(OH)67[7-], Sb[3+], SbOH[2+], Sb(OH)2[+] Sb(OH)4[-], Sb2(OH)6(s) Sb(c), Valentinite, Sb2O5(s)

HATCHES Sb(OH)3(aq), Sb[3+], Sb(OH)2[+], Sb(OH)4[-], Sb2O3

223

Sb (FACT/FACTSAGE)

Sb (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6 Sb2O4(s)

0.4

Eh(V)

0.4

Eh(V)

0.6

Sb2O5(s)

SbO[+] 0.2

0.0

HSbO2(aq)

0.2

0.0

SbO2[-]

HSbO2(aq) -0.2

-0.2

-0.4

SbO2[-]

Sb(s) -0.6

-0.4

-0.6

-0.8

-0.8 1

Sb (LLNL/GWB)

Sb (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Sb(OH)5(aq)

0.2

Eh(V)

Sb(OH)6[-]

NO DATA

Sb(OH)2[+] 0.2

0.0

-0.2

-0.4

-0.6

Sb(OH)3(aq)

-0.8

Sb(c)

Sb(OH)4[-]

-0.8 1

Figure 108: Eh-pH diagrams of the system Sb-O-H (1).

224

Sb = 10−10 , 298.15K, 105 Pa.

Sb (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Sb[3+]

Eh(V)

0.4 Sb(OH)3(aq)

0.2

0.0 Sb(OH)4[-] -0.2

-0.4

-0.6

-0.8 1

Figure 109: Eh-pH diagrams of the system Sb-O-H (2).

225

Sb = 10−10 , 298.15K, 105 Pa.

Table 68: List of Sc species FACT

SUPCRT

LLNL

Sc[3+], ScOH[2+], Sc[3+], ScOH[2+], ScO[+], HScO2(aq), Sc(s), Sc(s2), Sc2O3(s), Sc(OH)3(s) ScO2[-]

226

JNC-TDB

Sc (FACT/FACTSAGE)

Sc (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

0.2

Sc[3+]

ScOH[2+]

Eh(V)

Sc[3+]

Sc2O3(s)

HScO2(aq)

0.0

-0.2

-0.4

-0.6

-0.8 1

Sc (LLNL/GWB)

Sc (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

ScO2[-]

0.2

0.0

-0.8

ScO[+]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

0.2

-0.8 1

Figure 110: Eh-pH diagrams of the system Sc-O-H.

227

Sc = 10−10 , 298.15K, 105 Pa.

228

Table 69: List of Se species FACT HSe[-], SeO3[2-], SeO4[2-], HSeO3[-], H2SeO3(aq), HSeO4[], Se[2-], H2Se(aq), Se(s), SeO2(s), SeO3(s), Se2O5(s)

SUPCRT

LLNL

HSe[-], SeO3[2-], SeO3[2-], Se[2-], SeO4[2-], HSeO3[-], SeO4[2-], H2Se(aq), H2SeO3(aq), HSeO4[-] H2SeO3(aq), HSe[-], HSeO3[-], HSeO4[-], Se(black), Se2O5(s), SeO2(s), SeO3(s)

HATCHES SeO4[2-], Se[2-], SeO3[2-], H2Se(aq), H2SeO3(aq), HSe[-], HSeO3[-], HSeO4[-], Se, Se2O5, SeO2, SeO3

229

JNC-TDB SeO4[2-], Se[2-], HSe[-], H2Se(aq), SeO3[2-], HSeO3[-], H2SeO3(aq), HSeO4[], Se(s), SeO2(s), Se2O5(s), SeO3(s)

Se (FACT/FACTSAGE)

Se (SUPCRT/FLASK-AQ)

1.2

1.2 HSeO4[-]

HSeO4[-]

1.0

0.8

1.0

0.8

H2SeO3(aq)

0.6 HSeO3[-]

H2SeO3(aq)

0.4

Eh(V)

0.4

Eh(V)

0.6

SeO4[2-]

0.2 Se(s) 0.0

SeO4[2-]

HSeO3[-]

0.2

0.0

SeO3[2-]

HSe[-] -0.2

-0.4

-0.2 HSe[-]

H2Se(aq)

-0.4

-0.6

-0.8

-0.8 1

Se (LLNL/GWB)

1.2 HSeO4[-]

HSeO4[-] 1.0

1.0

0.8

0.8 H2SeO3(aq)

H2SeO3(aq) 0.6

0.6

SeO4[2-]

HSeO3[-]

0.4

Eh(V)

0.4

Eh(V)

Se (JNC-TDB/GWB)

1.2

0.2 Se(black) 0.0

0.2 Se(s) 0.0

SeO3[2-]

-0.2

-0.2 HSe[-]

-0.4

H2Se(aq)

-0.4

-0.6

H2Se(aq)

HSe[-]

-0.6

-0.8

-0.8 1

Figure 111: Eh-pH diagrams of the system Se-O-H (1).

230

Se = 10−10 , 298.15K, 105 Pa.

1.2

Se (HATCHES/FLASK-AQ) HSeO4[-]

1.0

0.8 H2SeO3(aq) 0.6

SeO4[2-] HSeO3[-]

Eh(V)

0.4

0.2 Se(s) 0.0

SeO3[2-]

H2Se(aq)

-0.2 HSe[-] -0.4

-0.6

-0.8 1

Figure 112: Eh-pH diagrams of the system Se-O-H (2).

231

Se = 10−10 , 298.15K, 105 Pa.

232

Table 70: List of Si species FACT

SUPCRT

H4SiO4(aq), HSi(OH)6[-], H2SiO3(aq), Si(s), Si2H5(s), H2SiO3(s), H4SiO4(s), H2Si2O5(s), H6Si2O7(s), SiO2(s), SiO2(s2), SiO2(s3), SiO2(s4), SiO2(s5), SiO2(s6), SiO2(s7), SiO2(s8)

SiO2(aq), HSiO3[-], SiO2(Amorpyoussilica), SiO2(Chalcedony), SiO2(Cristobalite, alpha), SiO2(Cristobalite, beta), SiO2(Coesite), SiO2(Cristobalite), SiO2(Quartz)

LLNL SiO2(aq), H2SiO4[2], H3SiO4[-], H4(H2SiO4)4[4-], H6(H2SiO4)4[2-], Amrph_silica, Chalcedony, Cristobalite, Quartz, Tridymite

JNC-TDB H4SiO4(aq), SiO2(OH)[2-], SiO(OH)3[-], Si2O3(OH)4[2-], Si2O2(OH)5[-], Si3O6(OH)3[3-], Si3O5(OH)5[3-], Si4O8(OH)4[4-], Si4O7(OH)5[3-], Si4O3(OH)13[3-], SiO2(s,Sil_gel), H2SiO3(s, Sil_glass), Chalcedony, Quartz, HSiO2(s, Silica_H), Sili(am), Si(c), SiO2(qua), Si(g)

HATCHES H4SiO4(aq), H2SiO4[2-], H3Si3O9[3-], H3SiO4[], H4Si2O7[2-], H4Si4O12[4-], H5Si2O7[-], H5Si3O10[3-], H5Si4O12[3-], Amrph.silica, Chalcedony, Cristobalite, Crist.beta, Quartz Remarks JNC-TDB: SiO2(qua) is not Quartz in the database file, its log10K's are different from those of Quartz, but detailed description of SiO2(qua) is not given.

233

Si (FACT/FACTSAGE)

Si (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4 H4SiO4(aq)

Eh(V)

0.4

0.2

SiO2(aq)

0.2

HSi(OH)6[-] 0.0

0.0

-0.2

-0.4

-0.6

HSiO3[-]

Si2H6(s) -0.8

-0.8 1

Si (LLNL/GWB)

Si (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.4 SiO2(aq)

Eh(V)

0.2

H4SiO4

0.2 SiO(OH)3[-]

H3SiO4[-] 0.0

0.0

H2SiO4[2-]

SiO2(OH)2[2-]

-0.2

-0.4

-0.6

-0.8

Silica_H

-0.8 1

Figure 113: Eh-pH diagrams of the system Si-O-H (1).

234

Si = 10−10 , 298.15K, 105 Pa.

1.2

Si (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Eh(V)

0.4 H4SiO4(aq)

0.2

0.0

H3SiO4[-]

-0.2 H2SiO4[2-] -0.4

-0.6

-0.8 1

Figure 114: Eh-pH diagrams of the system Si-O-H (2).

235

Si = 10−10 , 298.15K, 105 Pa.

236

Table 71: List of Sm species FACT Sm[2+], Sm[3+], Sm(s), Sm(s2), Sm2O3(s), Sm2O3(s2)

SUPCRT

LLNL

JNC-TDB Sm[3+], SmOH[2+], Sm(OH)2[+], Sm(OH)3(aq), Sm(OH)3(am), Sm(OH)3(c)

Sm[2+], Sm[3+], Sm[4+], SmOH[2+], SmO[+], SmO2H(aq), SmO2[-]

HATCHES Sm[3+], Sm(OH)2[+], Sm(OH)3(aq), SmOH[2+], Sm(OH)3

237

Sm (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.2

Sm[3+]

Sm2O3(s)

Eh(V)

Sm (FACT/FACTSAGE) 1.2

Sm[3+]

0.2 SmOH[2+]

0.0

0.0 SmO[+]

-0.2

-0.4

-0.6

-0.8

-0.8 1

Sm (LLNL/GWB)

Sm (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

SmO2[-]

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Sm[3+]

Sm(OH)2[+] Sm(OH)3(c) SmOH[2+]

-0.8 1

Figure 115: Eh-pH diagrams of the system Sm-O-H (1).

238

Sm = 10−10 , 298.15K, 105 Pa.

1.2

Sm (HATCHES/FLASK-AQ)

1.0

0.8

0.6

0.4

Eh(V)

Sm[3+]

0.2 SmOH[2+] 0.0 Sm(OH)3(aq)

-0.2

-0.4

-0.6

-0.8 1

Figure 116: Eh-pH diagrams of the system Sm-O-H (2).

239

Sm = 10−10 , 298.15K, 105 Pa.

240

Table 72: List of Sn species FACT Sn[2+], SnOH[+], SnO(OH)[+], Sn(s2), Sn(s), SnO(s), SnO2(s)

SUPCRT Sn[2+], SnOH[+], SnO(aq), HSnO2[-], Sn(Native tin), SnO(Romarchite), SnO2(Cassiterite)

LLNL

JNC-TDB

Sn[4+], Sn[2+], Sn(OH)2(aq), Sn(OH)2[2+], Sn(OH)3[+] Sn(OH)3[-], Sn(OH)4(aq), SnOH[+], SnOH[3+], Sn(OH)2(s), SnO(s), SnO2(s)

Sn(OH)4(aq), SnOH[+], Sn(OH)2(aq), Sn(OH)3[-], Sn3(OH)4[2+], Sn[2+] Sn(OH)5[-], Sn(OH)6[-], Sn[4+], Sn(c), Sn(OH)2(s), SnO(c), SnO2(am) SnO2(cassiterite)

HATCHES Sn[2+], Sn[4+], HSnO2[-], Sn(OH)[+], Sn(OH)2(aq), Sn(OH)2[2+], Sn(OH)3[+], Sn(OH)3[-], Sn(OH)4(aq), Sn(OH)5[-], Sn(OH)6[2-], Sn2(OH)2[2+], Sn3(OH)4[2+], SnOH[3+], H2Sn(OH)6, Sn(OH)2, Sn(OH)4, Sn(w), SnO, SnO2(am), SnO2(c), SnO2(pptd)

241

Sn (FACT/FACTSAGE)

Sn (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.6 SnO(OH)[+]

Eh(V)

0.4

Eh(V)

0.4

0.2

SnO2(s)

0.2

SnO2(s)

0.0

-0.2 Sn[2+]

-0.2 SnOH[+]

-0.4

Sn[2+] SnOH[+]

-0.4

SnO(aq) -0.6

-0.6

Sn(s)

Sn(s) -0.8

HSnO2[-]

-0.8 1

Sn (LLNL/GWB)

Sn (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Sn[4+]

Sn(OH)4(aq)

0.4

Eh(V)

Sn(OH)4(aq)

0.2

Sn(OH)5[-]

0.2

0.0

-0.2

Sn(OH)6[2-]

Sn[2+] -0.4

SnOH[+]

-0.4 Sn[2+] SnOH[+]

-0.6

Sn(OH)2(aq)

-0.6

Sn(OH)2(aq) -0.8 1

Sn(c) Sn(OH)3[-] 9 11

-0.8 13

Figure 117: Eh-pH diagrams of the system Sn-O-H (1).

242

Sn(OH)[-] 11

Sn = 10−10 , 298.15K, 105 Pa.

1.2

Sn (HATCHES/FLASK-AQ)

1.0

0.8

0.6 Sn(OH)2[++]

Eh(V)

0.4

Sn(OH)3[+] Sn(OH)4(aq)

0.2

0.0

Sn(OH)5[-]

-0.2 Sn[2+] Sn(OH)[+]

-0.4

-0.6

Sn(OH)2(aq)

Sn(w)

HSnO2[-]

-0.8 1

Figure 118: Eh-pH diagrams of the system Sn-O-H (2).

243

Sn = 10−10 , 298.15K, 105 Pa.

244

Table 73: List of Sr species FACT Sr[2+], SrOH[+], Sr(s), Sr(s2), SrH2(s), SrO(s), SrO2(s), Sr(OH)2(s)

SUPCRT Sr[2+], SrOH[+]

LLNL Sr[2+], SrOH[+], Sr(OH)2(c), SrO(c)

HATCHES Sr[2+], Sr(OH)2(aq), SrOH[+], Sr(OH)2, SrO(c)

245

JNC-TDB Sr[2+], SrOH[+], Sr(OH)2(aq), Sr(OH)2(s), Sr(c), SrO(c)

Sr (FACT/FACTSAGE)

Sr (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

0.2

Sr[2+]

SrOH[+]

Eh(V)

SrO2(s)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

SrOH[+]

-0.8 1

Sr (LLNL/GWB)

Sr (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Sr[2+]

SrOH[+]

Eh(V)

Sr[2+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Sr[2+]

SrOH[+]

-0.8 1

Figure 119: Eh-pH diagrams of the system Sr-O-H (1).

246

Sr = 10−10 , 298.15K, 105 Pa.

Sr (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

Eh(V)

0.4

0.2

Sr[2+]

0.0

SrOH[+]

-0.2

-0.4

-0.6

-0.8 1

Figure 120: Eh-pH diagrams of the system Sr-O-H (2).

247

Sr = 10−10 , 298.15K, 105 Pa.

Table 74: List of Tb species FACT Tb[3+], Tb(s), Tb(s2), TbO2(s), Tb2O3(s), Tb6O11(s), Tb7O12(s)

SUPCRT

LLNL

Tb[3+], Tb[4+], Tb[2+], TbOH[2+], TbO[+], TbO2H(aq), TbO2[-]

248

JNC-TDB

Tb (FACT/FACTSAGE)

Tb (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 TbO2(s)

0.8

0.6

0.4

0.4 Tb6O11(s)

Tb[3+]

Eh(V)

Tb[3+]

0.2 Tb7O12(s)

0.0

TbOH[2+] 0.2 TbO[+] 0.0

-0.2

TbO2H(aq) TbO2[-]

-0.2 Tb2O3(s)

-0.4

-0.6

-0.8

-0.8 1

Tb (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Tb (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 121: Eh-pH diagrams of the system Tb-O-H.

249

Tb = 10−10 , 298.15K, 105 Pa.

250

Table 75: List of Tc species FACT

SUPCRT

Tc(s), TcO2(s), TcO TcO4[-] 3(s), Tc2O7(s)

HATCHES

OECD-NEA

TcO[2+], Tc[3+], T TcO4[-], TcO4[2-], cO4[-], TcO(OH)[+], TcO4[3-], TcO(OH) TcO(OH)2(aq), TcO(O [+], TcO(OH)2(aq), H)3[-], HTcO4(s), T TcO(OH)3[-], Tc(c), c(c), Tc(OH)2, Tc(O TcO2(c), Tc2O7(c), T H)3, Tc2O7, Tc2O7*H2O, cO2*1.6H2O(s), Tc2O7 Tc3O4, Tc4O7, TcO2am, H2O(s) TcO21*6H2O, TcO3, T cOH

LLNL

JNC-TDB

TcO4[-], Tc[3+], TcO[2+], TcO4[2-], TcO4[3-], TcO(OH)2 (aq), TcOOH [+], [TcO(OH)2]2(a q), HTcO4(s), Tc(OH)2(s) Tc(OH)3(s), T c(c) Tc2O7(s), Tc3O4(s) Tc4O7(s), TcO2*2H2O (am) TcO3(s), TcOH(s)

TcO[2+], TcO4[2-], TcO4[-], TcO(OH)[+], TcO(OH)2(aq), TcO(O H)3[-], Tc(c), TcO2 (c), TcO216H2(s), Tc2 O7(c), Tc2O7H2O(s), Tc(g), TcO(g), Tc2O 7(g)

OECD-NEA update TcO4[-], TcO[2+], T cO4[2-], TcO(OH)[+], TcO(OH)2(aq), TcO (OH)3[-], Tc(cr), T cO2(cr), Tc2O7(cr), TcO2*1.6H2O(s), Tc2O 7H2O(s)

Remarks JNC-TDB: Given reaction of TcO216H2 in the database file suggests its formula as TcO3.6H3.2.

251

Tc (FACT/FACTSAGE)

Tc (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO AQUEOUS SPECIES DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Tc (LLNL/GWB)

Tc (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

TcO4[-]

0.2

TcO[2+]

0.6

TcOOH[+] 0.4

TcO4[-]

Tc3O4(s)

Eh(V)

0.4

0.2

0.0

TcO4[-]

TcO[2+] TcO(OH)[+]

0.0

-0.2

TcO(OH)2(aq)

-0.2

TcOH(s)

-0.4

-0.4 Tc(c) Tc(s)

-0.6

TcOOH3[-]

-0.6

-0.8

-0.8 1

Figure 122: Eh-pH diagrams of the system Tc-O-H (1).

252

Tc = 10−10 , 298.15K, 105 Pa.

1.2

Tc (OECD-NEA/FLASK-AQ)

Tc (HATCHES/FLASK-AQ)

1.2

1.0

0.8

0.6

0.6 TcO[2+]

TcO(OH)[+]

TcO(OH)[+] TcO4[-]

0.2

TcO4[-]

0.4

Eh(V)

0.4

0.2

Tc3O4(s)

0.0

TcO2(c)

Tc4O7(s) -0.2

-0.2

TcOH

-0.4

Tc(cr)

-0.4 TcO(OH)3[-] Tc(c)

-0.6

-0.8

-0.8 1

Tc (OECD-NEA update/FLASK-AQ) 1.2

1.0

0.8

0.6 TcO4[-]

Eh(V)

0.4 TcO[2+]

0.2 TcO2(cr)

0.0

-0.2

-0.4

TcO(OH)3[-] Tc(cr)

-0.6

-0.8 1

Figure 123: Eh-pH diagrams of the system Tc-O-H (2).

253

Tc = 10−10 , 298.15K, 105 Pa.

Table 76: List of Te species FACT

SUPCRT

LLNL

TeO3[2-], Te(OH)3[+], Te(s), TeO2(s), H2TeO4(s)

254

JNC-TDB

Te (FACT/FACTSAGE)

Te (SUPCRT/FLASK-AQ)

1.2

1.2 H2TeO4(s)

1.0

0.8

Te(OH)3[+]

0.6

0.4

Eh(V)

0.8

1.0

TeO3[2-]

0.2

0.0

NO DATA

0.2

0.0 Te(s)

-0.2

-0.4

-0.6

-0.8

-0.8 1

Te (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

0.2

Eh(V)

Te (LLNL/GWB)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

NO DATA

-0.8 1

Figure 124: Eh-pH diagrams of the system Te-O-H.

255

Te = 10−10 , 298.15K, 105 Pa.

256

Table 77: List of Th species FACT Th[4+], Th(s), Th(s2), ThH2(s), ThO2(s)

SUPCRT Th[4+]

LLNL Th[4+], Th(OH)2[2+], Th(OH)3[+], Th(OH)4(aq), Th2(OH)2[6+], Th4(OH)8[8+], Th6(OH)15[9+], ThOH[3+] Th(OH)4(c), ThO2(s), Thorianite

HATCHES Th[4+], Th(OH)[3+], Th(OH)2[2+], Th(OH)3[+], Th(OH)4(aq), Th2(OH)2[6+], Th4(OH)8[8+], Th(OH)4, ThO2,ThO2(c)

257

JNC-TDB Th[4+], Th(OH)4(aq), ThO2(am), ThO2(c)

Th (FACT/FACTSAGE) 1.2

1.0

0.8

0.6

0.6 Th[4+]

0.4

Eh(V)

0.4

Eh(V)

Th (SUPCRT/FLASK-AQ)

1.2

ThO2(s) 0.2

0.2 Th[4+]

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

1.2

1.0

0.8

0.6

0.4

0.2

Th (JNC-TDB/GWB)

1.2

Th[4+]

Eh(V)

Th (LLNL/GWB)

Thorianite

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Th[4+]

ThO2(c)

-0.8 1

Figure 125: Eh-pH diagrams of the system Th-O-H (1).

258

Th = 10−10 , 298.15K, 105 Pa.

1.2

Th (HATCHES/FLASK-AQ)

1.0

0.8

0.6

Th[4+]

Eh(V)

0.4

0.2

ThO2(c)

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 126: Eh-pH diagrams of the system Th-O-H (2).

259

Th = 10−10 , 298.15K, 105 Pa.

Table 78: List of Tl species FACT Tl[+], Tl[3+], TlOH(aq), TlOH[2+], Tl(OH)2[+], Tl(s), Tl(s2), Tl2O(s), Tl2O3(s), Tl2O4(s), TlOH(s), Tl(OH)3(s)

SUPCRT

LLNL

JNC-TDB Tl[+]

Tl[+], Tl[3+], TlOH(aq), TlOH[2+], TlO[+], HTlO2(aq), TlO2[-]

260

Tl (FACT/FACTSAGE)

Tl (SUPCRT/FLAKS-AQ)

1.2

1.0

1.0 Tl2O4(s)

0.6

0.4

0.2

Tl[+]

0.2

0.0

-0.2

-0.4

-0.6

-0.8

TlOH(aq)

-0.8 1

Tl (LLNL/GWB)

Tl (JNC-TDB/GWB)

1.2

1.0

0.8

0.6

0.4

Eh(V)

TlO2[-]

0.8

Eh(V)

0.8

HTlO2(aq)

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Tl[+]

-0.8 1

Figure 127: Eh-pH diagrams of the system Tl-O-H.

261

Tl = 10−10 , 298.15K, 105 Pa.

Table 79: List of Tm species FACT Tm[3+], Tm(s), Tm2O3(s), Tm2O3(s2), Tm2O3(s3)

SUPCRT

LLNL

Tm[3+], Tm[4+], Tm[2+], TmOH[2+], TmO[+], TmO2H(aq), TmO2[-]

262

JNC-TDB

Tm (FACT/FACTSAGE)

Tm (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

Tm[3+]

0.2

Tm[3+]

Eh(V)

1.2

Eh(V)

1.2

TmOH[2+]

0.2

Tm2O3(s)

0.0

-0.2

-0.4

-0.6

-0.8

TmO[+] TmO2H(aq)

TmO2[-]

-0.8 1

Tm (LLNL/GWB)

Tm (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 128: Eh-pH diagrams of the system Tm-O-H.

263

Tm = 10−10 , 298.15K, 105 Pa.

264

Table 80: List of U species FACT U[3+], U[4+], UO2 [+], UO2[2+], UOH[3 +], HO3U[+], H3O3U [+], H5O5U[-], H2O2U [2+], H2O6U2[2+], H5 O11U3[+], H7O13U3[-], U(s), U(s2), U(s3), UH3(s), UO3(s), U3O8 (s), U4O9(s), UO3(H2 O)(s), UO3(H2O)2(s), UO2(s)

SUPCRT

LLNL

JNC-TDB

U[4+], U[3+], UO2[+] U[4+], U[3+], UO2 U[3+], U[4+], UO2 [+], UO2[2+], UOH[3 UO2 UO2[2+], [+], [2+], UO2(OH)3(aq), (UO2)2(OH)2[2+], +], UO2OH[+], HUO2 UO2(OH)4(aq), (UO2)2 [+], HUO3[-], UOH[2 (UO2)3(OH)4[2+], OH(aq), (UO2)2(OH)2 +], UO[+], HUO2(aq), (UO2)3(OH)5[+], UO[2+], UO2(aq), U (UO2)3(OH)7[-],(UO2)4 [2+], (UO2)3(OH)4[2 +], (UO2)3(OH)5[+], O2OH(aq), UO3[-], U (OH)7[+], U(OH)2[2 U(OH)3 (UO2)3(OH)7[-], (UO2) O3(aq), HUO4[-], UO4 +], [2-], UO2(Uranitite) [+], U(OH)4(aq), U 4(OH)7[+], UO2OH[+], (OH)5[-], U6(OH)15[9 UO2(OH)2(aq), UOH[3 +], UO2OH[+], UOH[3 +], U(OH)4(aq), +], Gummite, Schoep UO2(am), UO3(alpha), UO3(beta), ite, U(c,alph), U3O UO3(gamma), UO3.0.9H, 8(c,alph), U4O9(c), UO2 UO2(OH)2(c,bet), UO2 UO3.2H2O, (am) UO3(c, (OH)2, U(c), UO2(c) gamma), Uraninite UO2.25(b), UO2.25(c), UO2.3333, UO2.6667, UH3 (beta), U(g), UO(g), UO2(g), UO3(g)

HATCHES

OECD-NEA

OECD-NEA update

U[4+], UO2[+], UO2 [2+], U(OH)[3+], U (OH)4(aq), U6(OH)15 [9+], Ul(OH)2(aq), Ul(OH)3[-], Ul(OH)4 [2-], Ul2(OH)2[2+], Ul2 OH[3+], Ul3(OH)4 [2+], Ul3(OH)5[+], Ul3 (O H)7[-], Ul4(OH) 7[+], UlOH[+], Gumm ite, Schoepite, U (c,alph), U3O8, U4O9, UO2(am), UO2(c), U O2(OH)2, UO2OH, UO3, UO3*2H2O, Uraninite

U[4+], U[3+], UO2 [+], UO2[2+], UOH[3 +], UO2OH[+], U(OH) 4(aq), UO2(OH) 3[-], UO2(OH)4[2-], (UO2)2 OH[3+], (UO2)2(OH)2 [2+], (UO2)3(OH)4[2 +], (UO2)3(OH)5[+], (UO2)3(OH)7[-], (UO 2)4(OH)7[+], U(c), UO2(c), UO2.25(c), UO 2.25(beta), UO2.3333(be ta), UO2.6667(c), UO3 (alpha), UO3(beta), UO3(gamma), UH3(bet a), UO3*0.9H2O(alph a), UO2(OH)2(beta), UO3*2H2O(c)

U[4+], U[3+], UO2 [+], UO2[2+], UOH[3 +], UO2OH[+], UO2(O H)2(aq), U(OH)4(aq), UO2(OH)3[-], UO2(OH) 4[2-], (UO 2)2OH[3+], (UO2)2(OH)2[2+], (UO 2)3(OH) 4[2+], (UO 2)3 (OH)5[+], (UO2)3(OH) 7[-], (UO2)4(OH) 7[+], U(cr), UO2(cr), UO 2.25(beta), UO2.25(cr), UO2.3333(beta), UO2.66 67(cr), UO3(alpha), UO3(beta), UO3(gamm a), UH3(beta), UO3* 0.9H2O(alpa), UO2(O H)2(beta), UO3*2H2O (cr)

Rmarks HATCHES: Ul stands for UO2. JNC-TDB: Given reaction of UO3.0.9H in the database file suggests its formula as UO3H. Given reaction of UO3.2H2O in the database file suggests its formula as UO3*2H2O. UO2.25(b) may be UO2.25(beta)?

265

U (FACT/FACTSAGE)

U (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.8 UO2[2+]

UO2[2+]

0.6

0.6 UO3(aq)

0.4

0.4 HUO4[-]

Eh(V)

H7O13U3[-]

0.2

0.2 UO4[2-] UOH[-3]

0.0

UO2(aq)

UO2[+] -0.2

-0.2 U[4+]

-0.4

UOH[3+]

-0.4 H5O5U[-] UO2(s)

-0.6 U[3+] -0.8

-0.8 1

UO2(s) 1

U (LLNL/GWB)

1.2

1.0

0.8

0.8 UO2[2+]

UO2[2+]

UO2OH[+]

0.6

0.4

Eh(V)

UO2(OH)2(aq)

0.4

(UO2)3(OH)7[-]

0.2

UO2(OH)3[-]

0.2

UO2[+]

U[4+]

0.0

U4O9(s) U[4+]

-0.2 UOH[3+]

-0.4

Uraninite U(OH)5[-]

-0.6

UO2(OH)4[2-]

UO2(cr)

-0.2

-0.4

U (JNC-TDB/GWB)

1.2

0.6

HUO3[-]

-0.6

UOH[3+]

-0.6 U[3+]

U[3+] -0.8

-0.8 1

Figure 129: Eh-pH diagrams of the system U-O-H (1).

266

U = 10−10 , 298.15K, 105 Pa.

U (OECD-NEA/FLASK-AQ)

U (HATCHES/FLASK-AQ) 1.2

1.2

1.0

0.8

0.8 UO2[2+] UO2[2+]

0.6

0.6 UO2OH[+] UO2(OH)4(aq)

0.4

Eh(V)

0.4

UO2(OH)3[-]

0.2

0.0

UO2(OH)3[-]

0.2

U[4+] U(OH)[3+]

UO2(OH)4[2-]

0.0

U[4+] UOH[3+] UO2(OH)4[2-]

-0.2

U(OH)4(aq)

-0.4

-0.6

-0.8

U(OH)4(aq)

U[3+] 1

U (OECD-NEA update/FLASK-AQ) 1.2

1.0

0.8

0.6 UO2(OH)2(aq)

UO2[2+] 0.4

Eh(V)

UO2OH[+]

0.2

0.0

UO2(OH)3[-]

U[4+] UOH[3+] UO2.25(cr)

UO2(OH)4[2-]

-0.2 UO2(cr) -0.4

-0.6 U[3+] -0.8 1

Figure 130: Eh-pH diagrams of the system U-O-H (2).

267

U = 10−10 , 298.15K, 105 Pa.

268

Table 81: List of V species FACT

SUPCRT

LLNL

VO[2+], VO2[+], VO4[3-], HVO4[2-], VO3[-], VO4[-], V2O7[4-], VOH2O2[3+], HVO4(aq), H2VO4[+], HV2O7[3-], H3V2O7[-], HV10O28[5-], H2V10O28[4-], V(s), VO(s), VO2(s), VO2(s2), V2O3(s), V2O4(s), V2O4(s2), V2O5(s), V3O5(s), V4O7(s)

VO[2+], VO2[+], VO4[3-], HVO4[2-], V[3+], V[2+], H3VO4(aq), H2VO4[-], VO[+], VOH[+], VOH[2+], VOOH[+]

V[3+], VO[2+], VO4[3-], (VO)2(OH)2[2+], (VO)2(OH)5[-], V(OH)2[+], V2(OH)2[4+], VO(OH)3(aq), VO2(OH)2[-], VO2[+], VO3OH[2-], VOH[2+], VOOH[+], V2O3(c), V2O4(c), V2O5(c), V3O5(c), V4O7(c)

HATCHES VO[2+], V[3+], VO2[+], VO4[3-], V2(OH)2[4+], VO(OH)[+], VO(OH)3(aq), VO)2(OH)2[2+], VO2(OH)2[-], VO3(OH)[2-], VOH[2+], V(OH)3, V2O3(c), V2O4(c), V2O5(c), V3O5(c), V4O7(c), VO(OH)2

269

JNC-TDB

V (FACT/FACTSAGE)

V (SUPCRT/FLASK-AQ)

1.2

1.0

1.0 VO2[+]

0.8

VO2[+] H3VO4(aq)

0.8 VO4[-]

0.6

H2VO4[-]

0.6 VO[2+]

0.2

VO3[-]

VO[2+]

VO4[3-]

0.2

0.0

VOOH[+]

V[3+] VOH[2+]

HVO4[2-] V3O5(s)

-0.2

HVO4[2-]

Eh(V)

0.4

Eh(V)

0.4

-0.2 VO[+]

-0.4

VO4[3-] V2O3(s)

-0.6

V[2+]

-0.6

VO(s) -0.8

VOH[+]

-0.8 1

V (LLNL/GWB)

V (JNC-TDB/GWB)

1.2

1.0

VO2[+] VO(OH)3(aq)

0.8

VO2(OH)2[-]

0.6

0.4

0.6

VO[2+]

0.4

Eh(V)

VO3OH[2-]

0.2

VO4[3-]

Eh(V)

1.0

0.2

0.0

-0.2

-0.2 V[3+]

-0.4

(VO)2(OH)5[-]

VOH[2+]

NO DATA

-0.4

V(OH)2[+] -0.6

-0.6 V2O3(s)

-0.8 1

-0.8 11

Figure 131: Eh-pH diagrams of the system V-O-H (1).

270

V = 10−10 , 298.15K, 105 Pa.

1.2

1.0

V (HATCHES/FLASK-AQ)

VO2[+]

0.8

VO(OH)3(aq)

0.6 VO2(OH)2[-] 0.4

Eh(V)

VO[2+]

0.2 V[3+]

VO3(OH)[2-]

VO(OH)[+]

0.0 VOH[2+] -0.2 V2O3(c)

-0.4

-0.6

-0.8 1

Figure 132: Eh-pH diagrams of the system V-O-H (2).

271

V = 10−10 , 298.15K, 105 Pa.

Table 82: List of W species FACT

SUPCRT

LLNL

WO4[2-], W(s), WO4[2-], HWO4[-] WO2(s), WO3(s), WO3(s2), O2W(OH)2(s)

272

JNC-TDB

W (FACT/FACTSAGE)

W (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4 O2W(OH)2(s)

Eh(V)

0.4

0.2

HWO4[-]

WO4[2-]

0.2

0.0

0.0 WO4[2-]

-0.2

WO2(s)

-0.2

-0.4

-0.4 W(s)

-0.6

-0.8

-0.8 1

W (LLNL/GWB)

W (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 133: Eh-pH diagrams of the system W-O-H.

273

W = 10−10 , 298.15K, 105 Pa.

Table 83: List of Y species FACT Y[3+], YOH[2+], Y2(OH)2[4+], Y(s), Y(s2), YH2(s), YH3(s), Y2O3(s), Y2O3(s2), YO3H3(s)

SUPCRT

LLNL

Y[3+], YOH[2+], YO[+], HYO2(aq), YO2[-]

274

JNC-TDB

Y (FACT/FACTSAGE)

Y (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

Eh(V)

0.4

Eh(V)

0.4

Y[3+]

0.2

YOH[2+]

0.2 YO[+]

Y(OH)[2+] 0.0

YO3H3(s)

-0.2

0.0

HYO2(aq)

-0.2 YO2[-]

-0.4

-0.6

-0.8

-0.8 1

Y (LLNL/GWB)

Y (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 134: Eh-pH diagrams of the system Y-O-H.

275

Y = 10−10 , 298.15K, 105 Pa.

Table 84: List of Yb species FACT Yb[2+], Yb[3+], Yb(s), Yb(s2), Yb2O3(s), Yb2O3(s2), Yb2O3(s3)

SUPCRT

LLNL

Yb[2+], Yb[3+], Yb[4+], YbOH[2+], YbO[+], YbO2H(aq), YbO2[-]

276

JNC-TDB

Yb (FACT/FACTSAGE)

Yb (SUPCRT/FLASK-AQ)

1.0

0.8

0.6

0.4

0.4 Yb[3+]

0.2

Yb[3+]

Eh(V)

1.2

Eh(V)

1.2

YbOH[2+]

0.2

0.0

-0.2

-0.4

-0.6

YbO2H(aq) YbO2[-]

-0.8

-0.8 1

Yb (LLNL/GWB)

Yb (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 135: Eh-pH diagrams of the system Yb-O-H.

277

Yb = 10−10 , 298.15K, 105 Pa.

278

Table 85: List of Zn species FACT

SUPCRT

Zn[2+], ZnO2[2-], Zn[2+], ZnO2[2-], ZnOH[+], HZnO2[-], ZnOH[+], HZnO2[-], Zn(OH)2(aq), ZnO(s), ZnO(aq), Zn(s), Zn(OH)2(s), ZnO(Zincite) Zn(OH)2(s2), Zn(OH)2(s3)

LLNL Zn[2+]

HATCHES Zn[2+], Zn(OH)2(aq), Zn(OH)3[-], Zn(OH)4[2-], Zn2(OH)6[2-], Zn2OH[3+], ZnO2[2], ZnOH[+],Zincite, Zn(OH)2

279

JNC-TDB

Zn (FACT/FACTSAGE)

Zn (SUPCRT/FLASK-AQ)

1.2

1.0

0.8

0.6

0.4

Zn[2+]

Eh(V)

Zn[2+]

0.2

Zn(OH)2(aq)

0.0

ZnOH[+]

0.0 HZnO2[-]

HZnO2[-]

-0.2

-0.2 ZnO2[2-]

-0.4

ZnO2[2-]

-0.6

-0.8

-0.8 1

Zn (LLNL/GWB)

Zn (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

Zn[2+]

0.2

NO DATA

0.2

0.0

-0.2

-0.4

-0.6

-0.8

-0.8 1

Figure 136: Eh-pH diagrams of the system Zn-O-H (1).

280

Zn = 10−10 , 298.15K, 105 Pa.

Zn (HATCHES/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

Eh(V)

Zn[2+]

0.2

Zn(OH)2(aq)

0.0 Zn(OH)3[-] -0.2 Zn(OH)4[2-] -0.4

-0.6

-0.8 1

Figure 137: Eh-pH diagrams of the system Zn-O-H (2).

281

Zn = 10−10 , 298.15K, 105 Pa.

282

Table 86: List of Zr species FACT ZrO[2+], Zr(s), Zr(s2), ZrH2(s), ZrO2(s), ZrO2(s2), ZrO2(s3)

SUPCRT

LLNL

JNC-TDB Zr(OH)4(aq), Zr(OH)5[-], ZrO2(am)

ZrO[2+], Zr[4+], ZrOH[3+], HZrO2[+], ZrO2(aq), HZrO3[-]

HATCHES Zr[4+], Zr(OH)[3+], Zr(OH)4(aq), Zr(OH)5[-], Zr3(OH)4[8+], Zr4(OH)8[8+], ZrO2(am), ZrO2(c)

283

Zr (SUPCRT/FLASK-AQ) 1.2

1.0

0.8

0.6

0.4

0.4 ZrO[2+]

0.2

ZrOH[3+]

Eh(V)

Zr (FACT/FACTSAGE) 1.2

ZrO[2+]

0.2

ZrO2(s)

0.0

HZrO2[+] ZrO2(aq)

0.0

HZrO3[-] -0.2

-0.2

-0.4

-0.6

-0.8

-0.8 1

Zr (LLNL/GWB)

Zr (JNC-TDB/GWB)

1.0

0.8

0.6

0.4

Eh(V)

1.2

Eh(V)

1.2

NO DATA

0.2

Zr(OH)4(aq)

0.2

0.0

-0.2

-0.4

-0.6

-0.8

Zr(OH)5[-]

-0.8 1

Figure 138: Eh-pH diagrams of the system Zr-O-H (1).

284

Zr = 10−10 , 298.15K, 105 Pa.

1.2

Zr (HATCHES/FLASK-AQ)

1.0

0.8

0.6 Zr(OH)[3+]

Eh(V)

0.4

0.2 ZrO2(c)

0.0

-0.2

-0.4

-0.6

-0.8 1

Figure 139: Eh-pH diagrams of the system Zr-O-H (2).

285

Zr = 10−10 , 298.15K, 105 Pa.