A Computer-Assisted Evaluation of the Thermochemical Data of the Compounds of Thorium

Home , Thorium compounds

& TECH NATX INST. OF 5TAND NIST REFERENCE

NBSIR 77-1300

D. D. Wagman, R. H. Schumm and V. B. Parker

Physical Chemistry Division Institute for Materials Research National Bureau of Standards Washington, D.C. 20234

August 1 977

r> ^rati for Qd, 3nal Atomic Energy Agency

f Standard Reference Data, NBS

/f77

NBSIR 77-1300

A COMPUTER-ASSISTED EVALUATION OF THE THERMOCHEMICAL DATA OF THE COMPOUNDS OF THORIUM

D. D. Wagman, R. H. Schumm and V. B. Parker

Physical Chemistry Division Institute for Materials Research National Bureau of Standards Washington, D.C. 20234

August 1977

Prepared for International Atomic Energy Agency and Office of Standard Reference Data, NBS

U.S. DEPARTMENT OF COMMERCE, Juanita M. Kreps, Secretary

Dr. Sidney Harman, Under Secretary

Jordan J. Baruch, Assistant Secretary for Science and Technology

NATIONAL BUREAU OF STANDARDS, Ernest Ambler, Acting Director

TABLE OF CONTENTS

I. General Description

1. Introduction 2

2. Explanation of the Contents of Tables 3

3. Unit of Energy and Fundamental Constants 8

4. Internal Consistency of the Tables 9

5. Arrangement of the Tables 11

II. Tables of Values for AHf% A3f° and S° at 298.15 K for

the Compounds of Thorium and the Reaction Catalog

III. Bibliography

IV. Appendix: Thermal Functions for Thorium Compounds A-1

Th(c,l) A-6

Th(g) ' A-7

ThO(g) A-8

ThO^Cc) A-9

Th02(g) A-10

ThF(g) A-11

ThF^Cg) A-12

ThF^(g) A-13

ThF^(c,l) A- 14

ThF^(g) A-15

ThCl(g) A- 16

ThCl2(g) A-17 ThCl^Cg) A-18

ThCl^ (c,l) A-19

ThCl^(g) A-20

ThBr(g) A-21

ThBr2(g) A-22

ThBr^Cg) A-23

ThBr^(c,l) k-lu,

ThBr^(g) A-25

Thl(g) ' \ A-26

Thl^Cg) A-27

ThIgCg) A-28

Thl^(c,l) A-29 A Computer-Assisted Evaluation of the Thermochemica 1 Data

of the Compounds of Thorium

by D. Wagman, R. Schumm, and V. B. Parker

Abstract

Selected values are given for the thermochemica 1 properties of

the compounds of thorium. They are obtained from a computer-assisted

least sums-least squares approach to the evaluation of thermodynamic data networks. The properties given, where data are available, are enthalpy of formation, Gibbs energy of formation, and entropy at

298.15 K (AHf°(298), AGf°(298), and S°(298)). The values are consistent with the CODATA Key Values for Thermodynamics. The reaction catalog from which this self consistent set of values is generated is given with a statistical analysis. Some thermal functions are also given, as well as detailed comments when necessary.

Kej^ords : Data evaluation; enthalpyj entropy; Gibbs energy; thermo-

chemical data networks; thermochemica 1 tables; thorium compounds.

1 .

I. General Description

1, Introduction

This report presents a computer-assisted comprehensive evaluation

of the thermocheraical properties of compounds of thorium at 298 K that

is consistent with the CODATA Key Values for Thermodynamics [75COD] .

A combined least sums-least squares technique previously described by

Garvin et al [76GAR/PAR] has been used. This computer-based evaluation

is an extension of the CATCH program developed by J. B. Pedley^ Univer-

sity of Sussex v7ho used linear least squares analysis on enthalpy

measurements [69GUE/PED]

Thorium represents the first complete analysis of an element and

its compounds to be done by this least sums-least squares approach to

the evaluation of thermodynamic data networks. A self consistent set

of values for Zfflf°, A?f°^ and S° is generated from the given reaction

catalog. A detailed analysis of the values leads us to believe that

they are as good as and as reliable as those which would be obtained

in the traditional sequential method. Comparisons of the performance

of the computer-assisted method used here versus the traditional

method are given in [76GAR/PAR],

A major advantage of this method is the rapid updating that is

possible when new data become available or if the interpretation of

the existing data must be revised. Another advantage of this method

is that a translation from one scale of auxiliary values (CODATA here)

to the NBS Technical Note 270 Scale or some other scale can be made

readily.

cL References are given in a chronologically ordered bibliography at the end of the report. They are cited in the text in coded form indicating year of publication and the first two authors. This report provides the following data: the final selceted values for /:^>Hf°, AGf" and S" for the compounds considered and their predicted reliabilities, the values used for auxiliary compounds, a catalog of the measurements upon which the solution is based, some newly developed thermal functions and, where, needed, comments on the interpretation of the data.

The values for properties of auxiliary compounds are either

CODATA selections [75COD] or compatible with them [75PAR/WAG].

The reaction catalog (following the selected values), from which the solution is derived, contains the set of experimental enthalpy,

Gibbs energy and entropy changes at 298 K as well as entropies at

298 K from low temperature Cp measurements or statistical calculations.

It also contains for each reaction the initial assigned uncertainty, the final weighting factor, the residual (i.e., the observed minus the predicted value), the standard deviation of the predicted value (95 per cent confidence level), a coded citation to the Bibliography, and, occasionally, brief comments on corrections made to or interpretation of individual measurements.

User^ of th'^ tables and reaction catalog are invited to comment on the selections, correct errors and bring new measurements to our attention.

2. Explanation of the Contents of the Tables

The following material provides definitions and conventions used in the tables.

3 :

2.1 Chemical Formulae and Physical States

The tables were reproduced from computer printout in which only capital (upper case) letters are available. Normal one-line chemical formulae are used^ with the following modifications:

Subscripts (counts of atoms) and superscripts (charge) are printed on line: TH'CL'4 = ThCl^; TH'CL'+3 = ThCl^

The apostrophe ' appears after each letter in a chemical sjmibol that would normally be written in lower case: TH'N = ThN

The centered dot^ used in hydrates and minerals^ is shown as a colon: TH'F4:2.5H20 = ThF, •2.5H^O 4 2

The physical state of the substance is appended to the chemical formula in parentheses: TH'CL'4(C) = ThCl^, crystalline

Conventions with respect to physical state are given in Table A.

2.2 Definition of S3mibols for Thermochemical Properties

The headings used in the tabulated Thermochemical Values have the following meanings

DELTA HF = zXEIf", standard enthalpy of formation at 298.15 K;

DELTA GF = Z^f°, standard Gibbs energy (formerly free energy), G, of formation at 298.15 K;

+/- SIGMA = Predicted reliability, "one sigma" (see paragraph 4.1)

In the reaction catalog the heading, PROP. MEAS. refers to

A3, and Z^S at 298 K for the process given; the S3mibols used are H, G, and S; the symbol S means S°2gg when it refers to a "process" written without reactants:

= TH'CL'4(C) S = 45.5 (standard entropy of cryst. ThCl,)

4 All H and G relationships are in kcal/mol; all S relationships in

cal/(mol'K).

All values refer to one mole of substance for the formula given.

2 . 3 Conventions Regarding Pure Substances

The values of the thermodynamic properties of the pure substances

given in these tables are for the substances in their standard states.

These standard states are defined as follows:

For a pure solid or liquid, the standard state at any temperature

is the substance in the condensed phase under a pressure of one atmosphere.

For a gas the standard state at any temperature is the hypothetical

ideal gas at unit fugacity, in which state the enthalpy is that of the

real gas at the same temperature and at zero pressure.

The phase of a substance is indicated in parentheses at the end

of the chemical formula. See Table A.

The values of AHf° and ASf given in the tables represent the

change in the appropriate thermodynamic quantity when one mole of

the substance in its standard state is formed, isothermally at the

indicated temperature, from the elements, each in its appropriate

standard reference state. The standard reference state at 298 K for

each element except phosphorus has been chosen to be the standard state

that is thermodynamically stable at 298 K and at one atmosphere pressure.

For phosphorus the standard reference state is the crystalline white

form; the more stable forms have not been well characterized thermo-

chemically. The same reference states have been maintained for the

5 elements at 0 K except for the liquid elements bromine and mercury for which the reference states have been chosen as the stable crystalline forms. The standard reference states for the elements are indicated in the tables by the fact that the values of /SHf° and

Zfif° are exactly zero.

The values of S° represent the virtual or "thermal" entropy of the substance in the standard state at 298.15 omitting contribu- tions from nuclear spins and isotopic mixing. Where data have been available only for a particular isotope^ they have been corrected when possible to the normal isotopic composition.

2 .4 Convention Regarding Solutions

For all dissolved substances the composition of the solvent is indicated in parentheses following the chemical formula. Except in

special cases ^ discussed below, the number of moles of the solvent associated with one mole of solute is stated explicitly. See Table A for the conventions used^

In some cases the concentration of the solute can not be specified.

These are indicated as "AU" (aqueous, unspecified) for water solutions and by "U" for non-aqueous and mixed media. In all these cases the solution may be assumed to be "dilute".

The standard state for a non-dissociated solute in aqueous solution is taken as the hypothetical ideal solution of unit molality, which has been designated as "std. state, m = 1", For strong electrolytes in aqueous solution the conventional standard state is the ideal

6 solution of unit activity (unit mean molality). The designation "A" is used for strong electrolytes in the standard state and "AO" for undissociated species in water solution. In non-aqueous media two standard states are commonly used. For the mole fraction scale,

"std. state, = I", x is added to the formula of the solvent. For the molal scale, "std, state, m = 1", either s or M is appended to the formula.

The value of Z\Hf° for a solute in its standard state is equal to the apparent molal enthalpy of formation of the substance in the infinitely dilute real solution, since the enthalpy of dilution of an ideal solution is zero. At this dilution the partial molal enthalpy is equal to the apparent molal quantity. At concentrations other than the standard state, the value of AHf° represents the apparent enthalpy of the reaction of formation of the solution from the elements comprising the solute, each in its standard reference state, and the appropriate total number of moles of solvent. In this repre-

sentation the value of AHf° for the solvent is not required. The experimental value for a heat of dilution is obtained directly as the

difference between the two values of AHf° at the corresponding concentrations. At finite concentrations the partial molal enthalpy of formation differs from the apparent enthalpy.

The values of the thermodynamic properties tabulated for the

individual ions in aqueous solution are based on the usual convention

7 that the values of AHf°, AGf", S" and Cp" for H*" (aq, std. state, m = 1) are zero. The properties of a neutral electrolyte in aqueous solution in the standard state are equal to the algebraic sum of these values for the appropriate kinds and numbers of individual ions assumed to constitute the molecule of the given electrolyte. For an

ionic aqueous species e.g., y ^^'^ properties tabulated refer to that undissociated ion, i.e. they are not equal to the sum of those for its constituent ions. By adopting the above convention with respect to aqueous H^, it follows that the thermodynamic relation

^f° = ^*'-T(^f° + n-0.5S''(H2)) holds for individual ionic species, with n equal to the algebraic value of the charge. For neutral electrolytes the normal consistency relationship applies. See section 4.

3. Unit of Energy and Fundamental Constants

All of the energy values given in these tables are expressed in terms of the thermochemical calorie. This unit, defined as equal to

4.184 joules exactly, is generally accepted for the presentation of chemical thermodynamic data. Values reported in other units have been converted to calories by means of the conversion factors for molecular energy given in Table B,

Values in this report are consistent with the CQDATA Fundamental

Constants [73COD].

The formula weights in the tables have been calculated from the molecular formula using the 1969 Table of Atomic Weights [70IUP].

8 Values are given to four decimal places for convenience in the computer processing.

4 . Internal Consistency of the Tables

The processes given in the reaction catalog have been obtained from the original articles^ using consistent values for all subsidiary and auxiliary quantities. The original data were corrected V7here possible for differences in energy units, molecular V7eights, temperature scales, etc. Thus we have sought to maintain a uniform scale of energies for all processes in the tables and catalog. In addition the final tabulated values of the properties of a substance satisfy all the known physical and thermodynamic relationships among these properties. The quantities AHf°, -AGf% and S° at 298.15 K satisfy the relation:

AGf° = AHf ° -TZ^f to the precision given. The special case of solutions is discussed in section 2.4. Furthermore the calculated value of any thennodynamic quantity for a reaction is independent of the path chosen for the evaluation.

4 . 1 Uncertainties

The uncertainty reported for a selected value is "one sigma" as developed in the final least squares solution of the reaction data base. The magnitude of the uncertainty reflects the overall fit of

the data in the entire network. It is not an estimate made by the data analyst based on how well various small sections of the network fit together. These uncertainties, when used in the usual "square root of sum of squares" formula overestimate the uncertainty of a process. This is because the selected values (answers) are highly correlated. Better estimates for processes that are in the data network are provided in the listing of the reaction catalog. These estimates allow for the correlations among values.

Since the selected values are computer generated, more places are given than may be warranted by the uncertainty. Although these extra figures in the absolute sense are not significant, the retention and use of these figures ensures that the experimental data from which these values are derived may be recovered with an accuracy equal to that of the original quantities. This is particularly important for enthalpies of solution, dilution and transition.

4.2 Relationship to Other Tables of Thermodynamic Properties

The chemical thermodynamic properties in the present table may be combined with those published by CODATA in order to calculate the change in a property for a process. However, we recommend against these values being combined with those in any other tabulation or with a property reported in an original research paper. In particular, we warn against indiscriminate combination with the NBS Technical

Note 270 Series. A conversion to the NBS Technical Note 270 Scale will be made and included in that series.

There are several reasons for avoiding the combination of thermochemical data from more than one table. The most important is that different large-scale tables use different thermochemical propei cies .10

- i

I of formation for substances that are ubiquitous in thermochemical measurements. Outstanding examples are in the common inorganic acids and their ions. Another reason is that the groups preparing different tables may have relied on different measurements as the basis for selecting property values.

It is difficult to predict a priori how a change in one selected formation property would affect values assigned to other substances because of the way these are linked by complex networks. In general^ it may be expected that the advantage of internal consistency of a table will be lost if values frcm several sources are combined and the experimental measurements may be reproduced poorly.

No general, simple algorithm can be suggested for overcoming this problem. If it becomes necessary to extend a table of data to substances other than those tabulated, the user is advised to consult the group that prepared the table about the procedure that he plans to use.

5 . Arrangement of the Tables

The compounds in the tables are entered according to the Standard

Order of Arrangement, (see Figure 1), by the principle of latest position. In this scheme, a compound is listed under the element occurring latest in the list; water of hydration is neglected. Within a given element^table will be found all of the compounds of that element with elements occurring earlier in the order; the arrangement within a table follows the same ordering.

11 STANDARD ORDER OF ARRANGEMENT

12 .

TABLE A ; Physical State Conventions

The following conventions are used to designate the physical state of a substance. These apply to the attached table and to the

NBS Thennochemica 1 Data Bank, This information appears in a parenthetical expression appended to the molecular formula. Some of the explanations imply a thermochemica 1 value^ particularly those for solutions. These normally are used in describing enthalpy measurements

Basic Symbols Explanation

(G) Gaseous, e.g., HCL' (G) for HCJ^(g)

(GS) Gaseous reference standard state for an element,

e.g., 02 (GS) for O^Cg)

(C) Crystalline, e.g., NH4CL' (C) for m^C^(c) (CS) Crystalline reference standard state for an element, e.g., RB'(CS) for Rb(c)

(L) Liquid, e.g., H20(L) for H20(i) (LS) Liquid reference standard state for an element.

e.g., BR'2(LS) for Br2('^) (AM) Amorphous

(GL) Glassy

(A) Hypothetical standard state of the ideal aqueous

solution at unit activity. For a neutral

electrolyte the value of a property is equal to

the algebraic sum of the values for the ions

assumed to constitute the molecule of the

electrolyte, e.g. HCL' (A) = ffl-(A) + CL'-(A). For

an ionic species this notation is commonly used to refer to the undissociated ion as written, e.g. HSOi-(A)

13 Symbol Explanation

(AO) Hypothetical standard state of the ideal aqueous

solution at unit activity of the undissociated

(non-ionized) species, e.g. HF(AO), HF2-(A0).

May also be used whenever the designation (A)

could be ambiguous. Note that the descriptions HS04-(A) and HSOi-(AO) are equivalent, but that HF(A) and HF(AO) are not.

(AU) Aqueous solution of undefined, but usually

dilute, concentration, e.g. XE'03(AU).

The sjnnbols used above occasionally are modified by numbers to distinguish two substances in the same state that have the same molecular

weight, as for isomers: (AU2) , (C3). They are also used in combination with descriptive material, e.g. (C:HE'), (C:AL') etc. to mean "crystalline, hexagonal", "crystalline, alpha form" etc.

Special notations for substances in solutions

The notations for the "state" of a substance in solution may combine a definition of the system, e.g. HC-^ in 220 moles of water, and a

specification of the thermochemical property associated with it.

Usually the thermochemical property is the apparent integral enthalpy

or free energy of formation or an absolute entropy, i.e. the formation

properties of the solvent are not included. If a partial molal property

is tabulated the notation D: ("D" for "differential") occurs as the

first term in the state bracket. The notations given below illustrate

the differences for integral and differential (partial molal) properties,

and extrapolated values. Examples are given for aqueous, mixed, and

non-aqueous solvents.

14 Symbol Explanat ion

HCL' (200H2O) An aqueous solution of specified composition,

e.g. one mole of HCjJ in 200 moles H2O. The

value of AHf represents the apparent integral

enthalpy of formation.

HCL' (D:2 00H2O) and These represent the partial molal (enthalpy) of H2O(D:HCL'+200H2O) formation of the substance in a solution of specified concentration, e.g. the partial molal

enthalpy of formation of HC^ and respectively,

in a solution consisting of 1 mole HCj^ and 200 moles H2O.

UCL'4(HCL'O^+50H20) This describes a solute dissolved in a mixed

solvent, e.g. one mole of VC£^ in a mixture of

1 mole of HCiO, and 50 moles H-0. The value of 4 2 Atlf represents the apparent integral enthalpy of

formation of the substance, UCi^, in the medium.

UCL'4(HCL'04+ This represents a solute at an unspecified but

50H20:AU) usually dilute concentration in a solvent mixture

of fixed composition.

15 1 1 — t 1 1 \11 1 1

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the Compounds of Thorium and the Reaction Catalog

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