Modeling cobalt (III) acetylacetonate and iron (III) acetylacetonate solubilities in supercritical CO2 with PC-SAFT based on experimentally-determined solid–liquid equilibria in organic solvents

A methodology to model the solubilities of metal complexes in supercritical CO2 is indispensable for effectively designing the supercritical CO2-based deposition method. Herein, the solubility of two metal acetylacetonates (acac), Co(acac)3 and Fe(acac)3, in supercritical CO2 was modeled based on the perturbed-chain statistical associating fluid theory (PC-SAFT) and experimentally-determined solid–liquid equilibria in organic solvents. This modeling approach is more predictive than conventional cubic-type equations of state or semi-empirical correlation models. The pure-component parameters of PC-SAFT for metal acetylacetonates are obtained by fitting the obtained solubility data to four typical organic solvents (toluene, acetone, 2-butanone, and ethyl acetate). By applying these PC-SAFT parameters, the model satisfactorily reproduced the solubilities of the metal complexes in supercritical CO2, particularly under low-temperature conditions even with the kij (binary interaction parameter) set to 0 in the combining rule. The isobaric solubilities can also be described by PC-SAFT by generalizing the temperature dependence of kij. [Display omitted] •Predictive PC-SAFT approach for metal acetylacetonates solubilities in scCO2.•PC-SAFT parameters determined by fitting newly measured solubilities in organic solvents.•PC-SAFT approach reproduces metal acetylacetonates solubilities in scCO2 without kij.•Generalized kij parameter improves calculated accuracies of isobaric and isothermal solubilities in scCO2.