Spreading fully at the ice-water interface is required for high ice recrystallization inhibition activity

Although materials for ice recrystallization inhibition (IRI) are essential for the cryopreservation of cells and tissues, there exists no guiding mechanism for the design of such materials. Therefore, the construction of materials for IRI relies on the try-and-error strategy. Herein, through changing the tacticity of hydroxyl groups on poly(vinyl alcohol) (PVA) backbones with the affinities of PVAs to ice unchanged, we experimentally find IRI activity decreases significantly for isotactic PVA in comparison to that of atactic PVA. Molecular dynamics simulation shows atactic PVA spreads fully at the ice-water interface due to its much stronger interaction with water. This indicates atactic PVA can cover more ice surface and possess a higher IRI activity when the same amount of PVAs are used, which is consistent with the results that PVA can cover the same amount of ice surface more efficiently through experimentally measuring the adsorption of PVAs on the ice surface. A guiding mechanism of high active IRI materials can be obtained: only having affinity to ice is not enough to obtain high IRI activity (i.e., only small amount of materials is required to reduce the size of ice crystals to ca. (35 +/- 10) mu m), IRI agents must also have high affinity to water, i.e., low interfacial energies, to both ice and water. The former is to guarantee the adsorption of the IRI agent on the ice surface, and the latter is required for the IRI agent to spread sufficiently at the ice-water interface. Therefore, each IRI molecule can effectively block the diffusion of water onto the ice surface, and consequently inhibits the growth of ice. A spreading coefficient of IRI agents is therefore introduced to quantitatively assess the capability of IRI agents to spread at the ice-water interface.