Bioinspired Control of Calcium Phosphate Liesegang Patterns Using Anionic Polyelectrolytes

The Liesegang phenomenon is a spontaneous pattern formation, which is a periodic distribution of the precipitate discovered in diffusion-limited systems. Over the past century, it has been experimentally attempted to control the periodicity of patterns and structures of precipitates by varying the concentration of the hydrogel or electrolytes, adding organic or inorganic impurities, and applying an electric or pH field. In this work, the periodic patterns of calcium phosphate were manipulated with an anionic macromolecular additive inspired by bone mineralization in which various noncollagenous proteins are involved in the formation of a polymer-induced liquid precursor. The periodic patterns were systematically controlled by adjusting the amount of poly(acrylic acid), and they were numerically simulated by adjusting the threshold concentration of nucleation. The change of the pattern is explained by improved stability and directional diffusion of the intermediate.