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Hygrometric measurements were made for {y Na 2 SO 4 + (1 − y) K 2 SO 4 }(aq) solutions for different ionicstrength fractions of Na 2 SO 4 with y = 0.2, 0.5, and 0.8 at 298.15 K and from total molalities of 0.2 mol•kg −1 to about the saturation of one of the solutes. From the experimental results, the osmotic coefficients are determined for different compositions of this system. The new Pitzer mixing ionic parameters are also calculated and used to predict the solute activity coefficients in this ternary solution. These results allow for the calculation of the excess Gibbs energy at total molalities for ionic-strength fractions y.