2018
DOI: 10.1073/pnas.1712911115
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Directed nucleation and growth by balancing local supersaturation and substrate/nucleus lattice mismatch

Abstract: Controlling nucleation and growth is crucial in biological and artificial mineralization and self-assembly processes. The nucleation barrier is determined by the chemistry of the interfaces at which crystallization occurs and local supersaturation. Although chemically tailored substrates and lattice mismatches are routinely used to modify energy landscape at the substrate/nucleus interface and thereby steer heterogeneous nucleation, strategies to combine this with control over local supersaturations have remai… Show more

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Cited by 28 publications
(27 citation statements)
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“…While no adsorption of sulfate ions onto the organics was detected, significant amounts of cation adsorption were measured (Table 1), which could increase the local dissolved cation concentration near the organic films (7,11,29). Typically, adsorbed ions on substrates, including inner-sphere and outer-sphere complexes, can form an electrical double layer (EDL) with a thickness of ∼1 nm (30,31).…”
Section: Resultsmentioning
confidence: 99%
“…While no adsorption of sulfate ions onto the organics was detected, significant amounts of cation adsorption were measured (Table 1), which could increase the local dissolved cation concentration near the organic films (7,11,29). Typically, adsorbed ions on substrates, including inner-sphere and outer-sphere complexes, can form an electrical double layer (EDL) with a thickness of ∼1 nm (30,31).…”
Section: Resultsmentioning
confidence: 99%
“…The results of XRD and Raman analyses demonstrate that the CaCO 3 precipitated on calcite (104) surfaces is calcite, whereas that formed on aragonite (110) surfaces is aragonite, which is attributed to the complete lattice match between minerals with identical phases [31,46]. The relative intensity of XRD reflections, as well as Raman frequencies, of the same type of substrate grown in different solutions is distinct, which is ascribed to different orientations of CaCO 3 precipitates on local surfaces.…”
Section: Different Crystallization Pathways Of Heterogeneous Nucleatimentioning
confidence: 93%
“…Based on classical nucleation theory, the energy barrier (∆G C ) to form a critical nucleus is positively correlated with γ 3 (∆Gc ∝ γ 3 /(−RTlnσ) 2 , where γ denotes the interfacial free energy, σ the supersaturation, and R and T represent gas constant and Kelvin temperature, respectively [30]. The precipitation rate is subsequently controlled by the lattice mismatch, because a larger lattice mismatch leads to a higher ∆G C [31].…”
Section: Introductionmentioning
confidence: 99%
“…Self-assembly processes that occur during biomineralization at ambient temperature afford highly functional materials with hierarchical architectures and stunning beauty that have prompted the development of rationally designed silicon-based materials. For example, silica-carbonate biomorphs comprised of encapsulated crystalline carbonate and amorphous silica have been synthesized by diffusing CO 2 into alkaline solutions of sodium silicate (affording CO 3 2− and H + ions) that results in the coprecipitation of SrCO 3 and SiO 2 [11][12][13][14][15][16][17] . This simple approach involves mixing of cheap ingredients (Na 2 SiO 3 and Sr/BaCl 2 ) to create silicon composites with unprecedented complex morphologies (vases, corals, flowers, worms and plates) that are generated through randomly dispersed growth processes 12,18 .…”
mentioning
confidence: 99%
“…These processes serve to create an artificial microenvironment that creates exactly the right chemical and thermodynamic conditions required for spatial control of the microstructures that are produced 25 . Initial reports into generating silica biomorph systems in dilute silica sols or silica gels involved immersion of a substrate into a solution containing reactive silicon precursors which resulted in the random generation of microstructures with no positional control 12,13,16,17 . More recently, a bubble mediated substrate water/ air interface strategy has been developed to induce crystallization at solid-liquid-gas triphasic contact lines that can be used to control the spatial arrangement and morphology of the self-assembled surfaces on polydimethylsiloxane (PDMS) surfaces 26 .…”
mentioning
confidence: 99%