Reactive Phase Equilibria in Silica Aerogel Synthesis: Experimental Study and Prediction of the Complex Phase Behavior Using the PC-SAFT Equation of State

Synthesis of silica aerogels can be markedly accelerated by adding carbon dioxide (CO2) during the sol−gel process. The optimization of the sol−gel process in the presence of CO2 requires the knowledge of the phase equilibrium of the reactants [tetraethyl orthosilicate (TEOS) and water (H2O)], the solvent, and CO2. The perturbed-chain statistical associating fluid theory (PC-SAFT) equation of state is applied here to investigate the conditions under which an undesirable liquid demixing of that quaternary reactive mixture occurs. In this work pure-component parameters of the PC−SAFT equation of state for the solvent acetonitrile (ACN) and TEOS have been identified. Binary interaction parameters of all six related binary systems were determined. The phase behavior of three systems, which are not available in the literature, were studied experimentally:  the vapor−liquid equilibria of the systems TEOS−CO2 and TEOS−ACN and the liquid−liquid equilibrium of the system ACN−H2O−TEOS. All four related ternary syst...