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. 2017 Mar 17;3(3):e1602285.
doi: 10.1126/sciadv.1602285. eCollection 2017 Mar.

Biomimetic mineral self-organization from silica-rich spring waters

Juan Manuel García-Ruiz  1 , Elias Nakouzi  2 , Electra Kotopoulou  1 , Leonardo Tamborrino  1 , Oliver Steinbock  2
Affiliations

Biomimetic mineral self-organization from silica-rich spring waters

Juan Manuel García-Ruiz et al. Sci Adv. .

Abstract

Purely inorganic reactions of silica, metal carbonates, and metal hydroxides can produce self-organized complex structures that mimic the texture of biominerals, the morphology of primitive organisms, and that catalyze prebiotic reactions. To date, these fascinating structures have only been synthesized using model solutions. We report that mineral self-assembly can be also obtained from natural alkaline silica-rich water deriving from serpentinization. Specifically, we demonstrate three main types of mineral self-assembly: (i) nanocrystalline biomorphs of barium carbonate and silica, (ii) mesocrystals and crystal aggregates of calcium carbonate with complex biomimetic textures, and (iii) osmosis-driven metal silicate hydrate membranes that form compartmentalized, hollow structures. Our results suggest that silica-induced mineral self-assembly could have been a common phenomenon in alkaline environments of early Earth and Earth-like planets.

Keywords: Aqua de Ney; Calcite; Chemical Gardens; Life detection; Prebiotic chemistry; Silica Biomorphs; nano composites; self-organization; witherite.

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Figures

Fig. 1
Fig. 1. Barium carbonate–based structures grown using the Ney water.
Smoothly curved biomorphic shapes (A and B), helical structures (C and D), and flat sheets (E) showing oscillatory features (F). (G and I) Higher-resolution images reveal the nanocrystals that constitute the biomorphs. (H) Nanocrystal alignment direction obtained from the correlation analyses of the micrograph in (G); inset shows a representative correlation map. (J and K) Some of the structures consist of nanowires. (L) Infrared spectrum shows silica (gray squares) and crystalline barium carbonate (black circles) peaks. (M) X-ray diffraction (XRD) diffractogram with the characteristic witherite peaks. a.u., arbitrary units. Scale bars, 50 μm (A), 200 μm (B), 10 μm (C), 2 μm (D), 20 μm (E and F), 1 μm (G and J), and 200 nm (I and K).
Fig. 2
Fig. 2. Calcium carbonate–based structures.
(A to D) Morphological trend from classical rhombohedra to nanostructured aggregates with increasing pH. (E to G) Scanning electron microscopy (SEM) image (F) of a crystal aggregate showing two distinctive morphologies and the Raman spectrum of the calcitic (E) and vateritic (G) domains of the crystal aggregate. (H and K) Hierarchical structures of stacked nanoplatelets consisting of nanoparticles. Scale bars, 20 μm (A and C), 5 μm (B, D, and F), 2 μm (H and I), 500 nm (J), and 50 nm (K).
Fig. 3
Fig. 3. Silica gardens.
(A to C) MSH tubular membranes produced by reaction of the Co salt pellet with the Ney water. (D) Comparative histogram of the chemical composition [energy-dispersive x-ray spectroscopy (EDX)] of the inner part (gray) and the outer part (black) of the Co-based tube. (E) Raman spectra of the Co-based tubes produced in Ney water (black) and laboratory sodium silicate (Sod. Sil.) solutions (gray). (F to H) MSH tubular membrane produced by the reaction of the Fe(II) salt pellet with the Ney water. (I) Comparative histogram for the chemical composition (EDX) of the inner part (gray) and the outer part (black) of the Fe-based tube. (J) Raman spectra of the Fe-based tubes produced in Ney water (black curve) and laboratory sodium silicate solutions (gray curve).
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