Abstract
Synergistic relations between organic molecules and mineral precursors regulate biogenic mineralization. Given the remarkable material properties of the egg shell as a biogenic ceramic, it serves as an important model to elucidate biomineral growth. With established roles of complex anionic biopolymers and a heterogeneous organic scaffold in egg shell mineralization, the present study explores the regulation over mineralization attained by applying synthetic polymeric counterparts (polyethylene glycol, poly(acrylic acid), poly(aspartic acid) and poly(4-styrenesulfonic acid-co-maleic acid)) as additives during remineralization of decalcified eggshell membranes. By applying Mg2+ ions as a co-additive species, mineral retrosynthesis is achieved in a manner that modulates the polymorph and structure of mineral products. Notable features of the mineralization process include distinct local wettability of the biogenic organic scaffold by mineral precursors and mineralization-induced membrane actuation. Overall, the form, structure and polymorph of the mineralization products are synergistically affected by the additive and the content of Mg2+ ions. We also revisit the physicochemical nature of the biomineral scaffold and demonstrate the distinct spatial distribution of anionic biomolecules associated with the scaffold-mineral interface, as well as highlight the hydrogel-like properties of mammillae-associated macromolecules.
Highlights
In higher organisms, biomineralization involves an efficacious integration of inorganic building units with an organic scaffold to yield functional materials [1,2,3]
Composite biominerals engineered by Nature exhibit remarkable formation routes and material properties
In the presence of certain charged additives, stabilized amorphous phases exhibit fluid- or gel-like properties, suggested in enabling homeostatic mineralization
Summary
Biomineralization involves an efficacious integration of inorganic building units with an organic scaffold to yield functional materials [1,2,3]. Several complex biominerals present an organic scaffold (or matrix), which plays a crucial role in regulating mineral growth by incorporating inorganic precursors, such as ions, ion-clusters and amorphous phases. In nacre and bone material, the physicochemical properties of the scaffold tune interactions with mineral precursors and subsequently lead to hierarchically-organized composite biominerals [3,7,8]. The niche conditions of crowding and confinement presented by the scaffold offer a defined physicochemical environment towards mineralization reactions [9,10]. The dynamism of additives with respect to conformation, charge, molar mass, self-association propensity and phase behavior in relation to the distinct stages of material formation are crucial for Inorganics 2017, 5, 16; doi:10.3390/inorganics5010016 www.mdpi.com/journal/inorganics
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