Biomorphs are a unique class of self-organised silica–carbonate mineral structures with elaborate shapes. This work presents first approaches to convert these inorganic architectures into organic/inorganic hybrids through silane chemistry, while maintaining the original structural complexity. Further functionality can be added by binding of metal nanoparticles or quantum dots or via local organic polymerisation at the carbonate surfaces.
Silica biomorphs are extraordinary inorganic superstructures formed via autocatalytic co‐precipitation and bottom‐up self‐assembly of alkaline‐earth carbonates and silica. However, they show no inherent functionality except for their striking textural motifs and curved morphologies. This work presents strategies to magnetize silica biomorphs, thus creating thermally stable ceramic microswimmers with unique elaborate shapes. This is achieved by growing super paramagnetic magnetite mesocrystals on and around the complex curved surfaces of biomorphs, while keeping their morphology and maintaining mesocrystal integrity. Selective mesocrystal formation on certain parts of the substrates is induced by chemical modification of the biomorph surface, increasing the loading of magnetite on the silica–carbonate structures and, in suitable cases, rendering them able to respond to external magnetic fields and move as microswimmer entities. In this way, the complex ultrastructure of silica biomorphs is successfully used as a template for functional ceramics. Furthermore, selective dissolution of the carbonate core from the biomorphs leads to hollow magnetic structures that could be filled with actives, thus serving as microcarriers with considerable loading capacity.
Crystallisation of barium carbonate in the presence of silica can lead to the spontaneous assembly of highly complex superstructures, consisting of uniform and largely co-oriented BaCO3 nanocrystals that are interspersed by a matrix of amorphous silica. The formation of these biomimetic architectures (so-called silica biomorphs) is thought to be driven by a dynamic interplay between the components, in which subtle changes of conditions trigger ordered mineralisation at the nanoscale. In particular, it has been proposed that local pH gradients at growing fronts play a crucial role in the process of morphogenesis. In the present work, we have used a special pH-sensitive fluorescent dye to directly trace these presumed local fluctuations by means of confocal laser scanning microscopy. Our data demonstrate the existence of an active region near the growth front, where the pH is locally decreased with respect to the alkaline bulk solution on a length scale of few microns. This observation provides fundamental and, for the first time, direct experimental support for the current picture of the mechanism underlying the formation of these peculiar materials. On the other hand, the absence of any temporal oscillations in the local pH - another key feature of the envisaged mechanism - challenges the notion of autocatalytic phenomena in such systems and raises new questions about the actual role of silica as an additive in the crystallisation process.
The formation of a polymer protection layer around fragile mineral architectures ensures that structures stay intact even after treatments that would normally destroy them going along with a total loss of textural information. Here we present a strategy to preserve the shape of silica-carbonate biomorphs with polymers. This method converts non-hybrid inorganic-inorganic composite materials such a silica/carbonate biomorphs into hybrid organic/carbonate composite materials similar to biominerals.
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