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Thermodynamic properties in the Fe(II)-Fe(III)-As(V)-HClO4–H2O and Fe(II)-Fe(III)-As(V)-HCl–H2O systems from 5 to 90 °C

Chemical Geology
By: , , , , and 
https://doi.org/10.1016/j.chemgeo.2017.04.010

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Abstract

Fe-As mineral solubility and associated aqueous species have been intensively studied because of the environmental need to immobilize arsenic. The thermodynamic data for aqueous iron-arsenic species are inadequately characterized, however. The Gibbs free energy, enthalpy, entropy, and heat capacity and activity coefficients were refined in the Fe(II)-Fe(III)-As(V)-HClO4-H2O and Fe(II)-Fe(III)-As(V)-HCl-H2O systems using redox potential measurements from 5 to 90 °C. The association constants for FeHAsO4+ and FeH2AsO42 + at 25 °C were 1010.28 and 104.02 and the corresponding association reaction enthalpies and heat capacities were 25.74 and 8.73 kJ mol− 1 and 843.1 and − 529.6 J K −1mol− 1, respectively. Activity coefficients for H+, ClO4−, Fe2 +, Fe3 +, HAsO42 −, and H2AsO4− at 25 °C in the form of the Hückel equation were derived for ionic strengths up to 1 mol− 1 kg− 1. Newly derived activity coefficients and thermodynamic data were incorporated into PHREEQCI to calculate the Eh of laboratory solutions. The differences between calculated and measured Eh were all within 10 mV and relative differences were all lower than 1.5%.

    Publication type Article
    Publication Subtype Journal Article
    Title Thermodynamic properties in the Fe(II)-Fe(III)-As(V)-HClO4–H2O and Fe(II)-Fe(III)-As(V)-HCl–H2O systems from 5 to 90 °C
    Series title Chemical Geology
    DOI 10.1016/j.chemgeo.2017.04.010
    Volume 460
    Year Published 2017
    Language English
    Publisher Elsevier
    Contributing office(s) Volcano Science Center
    Description 9 p.
    First page 37
    Last page 45
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