Chemical trigger toward phase separation in the aqueous Al(III) system revealed

Lukić, Miodrag J.; Wiedenbeck, Eduard; Reiner, Holger; Gebauer, Denis

doi:10.1126/sciadv.aba6878

Cited by 19 publications

(12 citation statements)

References 32 publications

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“…In the case of the PNC pathway, the event of phase separation then does not rely on overcoming a certain critical size (nucleation barrier, or level of supersaturation) as in CNT (Figure 1, top), but rather on a distinct decrease in their structural and/or configurational dynamics upon coordination or chemical changes occurring within the clusters. [17,[19][20][21][22] Hereby, phase separation does not occur spontaneously from PNCs due to significant barriers associated with further dehydration. [23] This provides an answer to the above question: Stable solute clusters (PNCs) can participate in phase separation when they undergo subtle changes in structure, slowing down the cluster dynamics.…”

Section: G Rtmentioning

confidence: 99%

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Gebauer

Gale

Cölfen

2022

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In this review article, selected, latest theoretical, and experimental developments in the field of nucleation and crystal growth of inorganic materials from aqueous solution are highlighted, with a focus on literature after 2015 and on non‐classical pathways. A key point is to emphasize the so far underappreciated role of water and solvent entropy in crystallization at all stages from solution speciation through to the final crystal. While drawing on examples from current inorganic materials where non‐classical behavior has been proposed, the potential of these approaches to be adapted to a wide‐range of systems is also discussed, while considering the broader implications of the current re‐assessment of pathways for crystallization. Various techniques that are suitable for the exploration of crystallization pathways in aqueous solution, from nucleation to crystal growth are summarized, and a flow chart for the assignment of specific theories based on experimental observations is proposed.

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Section: G Rtmentioning

confidence: 99%

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Gebauer

Gale

Cölfen

2022

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“…The results presented here pushes our current understanding of the formation of amorphous mineral phases further towards a particle self-assembly process starting from complex solute species, and correlates with recent observations in other inorganic systems. 37 The novel combination of methods allows for exploring the mesoand ultrastructure of ACC in response to specific synthesis conditions and the impact of reaction conditions on the chemical and isotopic composition of biominerals 8 . This unprecedented level of comprehensive ultrastructural information enables more accurate structural modelling of the major interaction partners and better mechanistic insight into the genesis of amorphous and crystalline solid-state materials from solutions.…”

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confidence: 99%

Nano- and Mesoscale Structures of Amorphous Calcium Carbonate Indicate Nanoscale Assembly Processes

Clark¹,

Colas²,

Jacob³

et al. 2021

Preprint

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<div>Here, we approach the issue of ACC ultrastructure by applying a method for determining atomically resolved structures of amorphous materials using Monte Carlo simulations constrained by both X-ray and neutron scattering data. This structural analysis approach allows us to develop a detailed model for ACC at the atomic level. Our findings reveal that synthetic ACC, rapidly precipitated at high pH, consists of two-nanometer sized units containing a high degree of near range order similar to partially disordered nano-crystals. Small-angle scattering analyses show a multi-scale hierarchical organisation of the structure, supportive of a multi-step colloid self-assembly process. Computer simulations and high-resolution transmission electron microscopy show that the mesostructure of ACC resembles that of a glassy gel with crystalline material in domains. Our findings support the formation of ACC by a nanoparticle aggregation process that likely starts from prenucleation clusters in solution.</div>

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“…Although this Perspective focuses on the minerals presented in biominerals, MBSMs consisting of other minerals, such as alumina, could also be fabricated via matrix-directed mineralization. Efforts have been made to understand the mineralization of other minerals, − yet more explorations are needed to make MBSMs based on these minerals.…”

Section: Discussion and Future Perspectivementioning

confidence: 99%

Matrix-Directed Mineralization for Bulk Structural Materials

Mao

Meng

et al. 2022

J. Am. Chem. Soc.

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Mineral-based bulk structural materials (MBSMs) are known for their long history and extensive range of usage. The inherent brittleness of minerals poses a major problem to the performance of MBSMs. To overcome this problem, design principles have been extracted from natural biominerals, in which the extraordinary mechanical performance is achieved via the hierarchical organization of minerals and organics. Nevertheless, precise and efficient fabrication of MBSMs with bioinspired hierarchical structures under mild conditions has long been a big challenge. This Perspective provides a panoramic view of an emerging fabrication strategy, matrix-directed mineralization, which imitates the in vivo growth of some biominerals. The advantages of the strategy are revealed by comparatively analyzing the conventional fabrication techniques of artificial hierarchically structured MBSMs and the biomineral growth processes. By introducing recent advances, we demonstrate that this strategy can be used to fabricate artificial MBSMs with hierarchical structures. Particular attention is paid to the mass transport and the precursors that are involved in the mineralization process. We hope this Perspective can provide some inspiring viewpoints on the importance of biomimetic mineralization in material fabrication and thereby spur the biomimetic fabrication of high-performance MBSMs.

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Chemical trigger toward phase separation in the aqueous Al(III) system revealed

Cited by 19 publications

References 32 publications

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Nano- and Mesoscale Structures of Amorphous Calcium Carbonate Indicate Nanoscale Assembly Processes

Matrix-Directed Mineralization for Bulk Structural Materials

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