Freezing-Memory Effect of Water on Nucleation of CO₂ Hydrate Crystals

Abstract

We measured the times to nucleate CO2 hydrates from CO2 dissolved water under pressure and 8.6 K supercooling using different methods to prepare the water. These times ranged from 50 min to more than 7200 min, depending on the preparation method. The nucleation rates were calculated by fitting the observed nucleation probability distributions to a nucleation rate equation. The nucleation rates significantly increased when the water had previously frozen as ice and melted (freezing-memory effect), except when the meltwater was heated to 298 K before nucleation. The nucleation rates also increased with O2-saturated meltwater, but decreased with degassed water.