INTRODUCTION



With the increase in the amount of thermodynamic data available for common minerals (Robie and Waldbaum, 1968; Stull and Prophet, 1971), it has become possible to calculate chemical equilibrium in multicomponent geological environments. Previously phase equilibria had to be measured in the laboratory using complicated equipment, which involved considerable time and cost. The same results can be obtained by the use of computers and available thermodynamic data. Various approaches to tills problem have been used by Lord (1965), Smith (1965, 1966), Helgeson (1969, 1970), Kaufman and Bernstein (1970), Skippen (i970), Griffiths et al (1972), Grossman (1972), and Zen (1972).

Zeleznik and Gordon (1962) wrote a computer program to compute chemical equilibrium compositions, rocket performance, and Chapman-Jouquet detonations. This program was modified and updated by Gordon and McBride (1971) to include incident and reflected shocks and is the basis of this study. The program was modified to facilitate calculation of solid-vapor equilibria at a given pressure and temperature for many types of geological systems as well as cosmic systems. Changes were made to include fugacity coefficients of gases, molar volumes of solids and to consider all possible species. Once the program had been modified and was operational, test cases were run consisting of systems, which had been studied experimentally. This study included a one-component system (SiO2), binary systems (MgO-SiO2; MgO-H2O; CaO-SiO2; CaO-H2O; MgO-CO2), ternary systems (MgO-CO2-H2O; MgO-H2O-N2), and metamorphic systems (tremolite-H2O-CO2; tremolite-H2O). The calculations compared favorably with the experimental results. This means that, with reliable thermodynamic data, a considerable amount of time could be saved in the laboratory by the use of a computer program.





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Table 1.-- List of symbols.


Symbol
Description
ai
Least squares coefficients (i = 1 to 7).
aij
Stotchiometric coefficient of element i of species j.
a
Integration constant.
boi
Assigned Kg-atoms of element i per Kg of total reactant (Kg-atom)i / Kg.
bi
Kg-atoms of element i per Kg of mixture, (Kg-atom)i / Kg.
Cp
Heat capacity in calories.
(Cpo)j
Standard state constant pressure specific heat for species or reactant j.
Gj
μj / RT, dimensionless Gibbs free energy for species j.
Gto
Gibbs free energy at temperature T.
ΔGfo
Gibbs free energy of formation from reference state.
Ht
Heat content in kilocalories.
Hj
(Hot)j / RT, dimensionless enthalpy for species j.
(Hto)j
Enthalpy of reactant j.
ΔH298o
Heat of formation from reference state.
L
Number of chemical elements in the system.
m
Number of possible gaseous species.
N
Total number of possible species.
n
Moles of mixture.
nj
Kg-moles of species j per Kg of mixture.
P
Pressure in bars.
R
Universal gas constant.
S
Entropy of species j.




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Table 1.-- (Continued).


Symbol
Description
St
Entropy in calories.
(Sot)j
Standard state entropy for species j.
T
Temperature in degrees Kelvin.
μj
Chemical potential of species j.
Vj
Molar volume of species j.
λ
Control factor used to limit size of corrections to original estimates.
πi
Lagrangian multiplier for chemical element i.
γ
Fugacity coefficient.




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