Multistep nucleation of nanocrystals in aqueous solution

Loh, N. Duane; Sen, Shamik; Bosman, Michel; Tan, Shu Fen; Zhong, Jun; Nijhuis, Christian A.; Král, Petr; Matsudaira, Paul; Mirsaidov, Utkur

doi:10.1038/nchem.2618

Cited by 346 publications

(422 citation statements)

References 37 publications

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“…In general, amorphous materials as the most unstable solid states would typically transform into more stable crystalline phases. 2,3 In the case of calcium carbonate, for example, amorphous calcium carbonate (ACC) has been widely observed as a transient precursor for the formation of crystalline calcium carbonate biominerals. 4 Here, we report that the opposite transformation from a crystalline calcium carbonate phase into ACC can also happen spontaneously.…”

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confidence: 99%

Reentrant phase transformation from crystalline ikaite to amorphous calcium carbonate

et al. 2018

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We report the spontaneous transformation of highly hydrated crystalline ikaite into less hydrated amorphous calcium carbonate (ACC), which has the outer contours of micrometer-sized crystals, a multi-level interconnected porous structure and a very high specific surface area (98.3 cm 2 g −1 ). 4 Here, we report that the opposite transformation from a crystalline calcium carbonate phase into ACC can also happen spontaneously. Solid state amorphization, a process where a crystalline phase transforms into an amorphous state, may happen through a large input of energy necessary for such an energetically "uphill" conversion of structures. A typical example is mechanical grinding of crystalline materials, which may lead to amorphous materials via generation of localized heating followed by quenching, via an increase in disorder or massive creation of defects. . The SEM images of ACC (d) and a sample during transformation (∼2400 s, ACC + ikaite) (e).

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Reentrant phase transformation from crystalline ikaite to amorphous calcium carbonate

et al. 2018

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“…Solidification via crystallization is the seminal procedure controlling the processing of virtually all metals and alloys in use today, yet controlled crystallization can be utilized as a prototypical self‐assembly strategy for synthesizing patterned structures across multiple length‐scales. The centrality of crystallization phenomena in many scientific fields has spurred decades of research into this “secretive” process. By tuning the growth conditions, it is possible to steer the system down different kinetic pathways to produce transient or metastable states (e.g., polytetrahedral or disordered phases) on intermediate time–scales .…”

Section: Introductionmentioning

confidence: 99%

Multi‐Step Crystallization of Self‐Organized Spiral Eutectics

Moniri

Bale

Volkenandt

et al. 2020

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A method for the solidification of metallic alloys involving spiral self‐organization is presented as a new strategy for producing large‐area chiral patterns with emergent structural and optical properties, with attention to the underlying mechanism and dynamics. This study reports the discovery of a new growth mode for metastable, two‐phase spiral patterns from a liquid metal. Crystallization proceeds via a non‐classical, two‐step pathway consisting of the initial formation of a polytetrahedral seed crystal, followed by ordering of two solid phases that nucleate heterogeneously on the seed and grow in a strongly coupled fashion. Crystallographic defects within the seed provide a template for spiral self‐organization. These observations demonstrate the ubiquity of defect‐mediated growth in multi‐phase materials and establish a pathway toward bottom‐up synthesis of chiral materials with an inter‐phase spacing comparable to the wavelength of infrared light. Given that liquids often possess polytetrahedral short‐range order, our results are applicable to many systems undergoing multi‐step crystallization.

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“…Mirsaidov and colleagues have observed AuNP formation dynamics with TEM. 32 Initially, gold is homogeneously spread throughout the solution.…”

Section: Discussionmentioning

confidence: 99%

On the mechanism of protein-templated gold nanoparticle synthesis: Protein organization, controlled gold sequestration, and unexpected reaction products.

Hart¹,

Abuladel²,

Bee³

et al. 2017

Preprint

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Emerging applications that exploit the properties of nanoparticles for biotechnology require that the nanoparticles be biocompatible or support biological recognition. These types of particles can be produced through syntheses that involve biologically relevant molecules (proteins or natural extracts, for example). Many of the protocols that rely on these molecules are performed without a clear understanding of the mechanism by which the materials are produced. We describe a single-pot reaction in which protein-templated gold nanoparticles (AuNPs) are produced as either solution-suspended colloids or as colloids formed within a solid, fibrous protein structure. We have investigated the mechanism for this process by detailing the reaction kinetics and outcomes through the use of 7 different proteins over a range of concentrations and temperatures. The key factor that controls the synthetic outcome (colloid or fiber) is the concentration of the protein relative to the gold concentration. We find that the observed fibrous structures are more likely to form at low protein concentrations and when hydrophilic proteins are used.An analysis of the reaction kinetics shows that AuNP formation occurs faster at lower protein (fiber-forming) concentrations than at higher protein (colloid-forming) concentrations. These results contradict expectations for reaction kinetics and proteinfiber formation, highlighting the need for a better understanding of the mechanism by which biomolecules can facilitate nanoparticle synthesis. As the protein properties that influence this mechanism are better recognized, researchers will be able to better utilize proteins to generate geometry-controlled AuNPs.

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Multistep nucleation of nanocrystals in aqueous solution

Cited by 346 publications

References 37 publications

Reentrant phase transformation from crystalline ikaite to amorphous calcium carbonate

Reentrant phase transformation from crystalline ikaite to amorphous calcium carbonate

Multi‐Step Crystallization of Self‐Organized Spiral Eutectics

On the mechanism of protein-templated gold nanoparticle synthesis: Protein organization, controlled gold sequestration, and unexpected reaction products.

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