Formation, Chemical Evolution, and Solidification of the Calcium Carbonate Dense Liquid Phase

DeYoreo, James J.; Jin, Biao; Chen, Ying; Pyles, Harley; Baer, Marcel D.; Legg, Ben; Wang, Zheming; Washton, Nancy M.; Mueller, Karl T.; Baker, David; Schenter, Gregory K.; Mundy, Christopher J.

doi:10.21203/rs.3.rs-1743346/v1

Cited by 4 publications

(2 citation statements)

References 24 publications

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“…The process of nucleation in complex solutions may be dependent upon chemical reactions and changes in species stoichiometry occurring locally. Several studies [50][51][52] have attributed the multi-step nature of nucleation to these factors. Simulating reactive crystallization events is often beyond the scope of classical molecular simulations using semiempirical, non-reactive force fields.…”

Section: Single-step Versus Multi-step Nucleationmentioning

confidence: 99%

Molecular simulation approaches to study crystal nucleation from solutions: Theoretical considerations and computational challenges

Finney,

Salvalaglio

2023

WIREs Comput Mol Sci

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Nucleation is the initial step in the formation of crystalline materials from solutions. Various factors, such as environmental conditions, composition, and external fields, can influence its outcomes and rates. Indeed, controlling this rate‐determining step toward phase separation is critical, as it can significantly impact the resulting material's structure and properties. Atomistic simulations can be exploited to gain insight into nucleation mechanisms—an aspect difficult to ascertain in experiments—and estimate nucleation rates. However, the microscopic nature of simulations can influence the phase behavior of nucleating solutions when compared to macroscale counterparts. An additional challenge arises from the inadequate timescales accessible to standard molecular simulations to simulate nucleation directly; this is due to the inherent rareness of nucleation events, which may be apparent in silico at even high supersaturations. In recent decades, molecular simulation methods have emerged to circumvent length‐ and timescale limitations. However, it is not always clear which simulation method is most suitable to study crystal nucleation from solution. This review surveys recent advances in this field, shedding light on typical nucleation mechanisms and the appropriateness of various simulation techniques for their study. Our goal is to provide a deeper understanding of the complexities associated with modeling crystal nucleation from solution and identify areas for further research. This review targets researchers across various scientific domains, including materials science, chemistry, physics and engineering, and aims to foster collaborative efforts to develop new strategies to understand and control nucleation.This article is categorized under: Molecular and Statistical Mechanics > Molecular Dynamics and Monte‐Carlo Methods Molecular and Statistical Mechanics > Free Energy Methods Theoretical and Physical Chemistry > Statistical Mechanics

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Section: Single-step Versus Multi-step Nucleationmentioning

confidence: 99%

Molecular simulation approaches to study crystal nucleation from solutions: Theoretical considerations and computational challenges

Finney,

Salvalaglio

2023

WIREs Comput Mol Sci

View full text Add to dashboard Cite

show abstract

“…The process of nucleation in complex solutions may be dependent upon chemical reactions and changes in species stoichiometry occurring locally. Several studies [47,48,49] have attributed the multi-step nature of nucleation to these factors. Simulating reactive crystallization events is often beyond the scope of classical molecular simulations.…”

Section: Single-step Vs Multi-step Nucleationmentioning

confidence: 99%

Theoretical and computational approaches to study crystal nucleation from solution

Finney

Salvalaglio

2023

Preprint

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Nucleation is the initial step towards the formation of crystalline materials from solutions. Various factors, such as environmental conditions, additives, and external forces, can influence its outcomes and rates. Indeed, controlling this rate-determining step towards phase separation can affect the material structure and properties, and it is crucial in a range of scientific fields. In this regard, atomistic simulation methods can be exploited to gain insight into nucleation mechanisms - an aspect difficult to ascertain in experiments - and estimate nucleation rates. However, the microscopic nature of simulations affects the phase behaviour of nucleating solutions when compared to macroscopic systems. Additionally, a challenge in modelling nucleation from solution is associated with the inadequacy of standard molecular simulations to access the timescales necessary to observe crystal nucleation due to the inherent rareness of these events. In recent decades, simulation methods have emerged to circumvent length- and timescale limitations. However, which simulation method is most suitable for studying crystal nucleation from solution is not always obvious. This review summarises the recent advances in this field, providing an overview of the typical nucleation mechanisms and the suitability of different simulation methods to study them. By doing so, we aim to provide a deeper understanding of the complexities associated with modelling crystal nucleation from solution and identify areas for further research. Our review targets researchers across various scientific fields, including materials science, chemistry, physics and engineering, and will hopefully contribute to developing new strategies for understanding and controlling nucleation.

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Directing polymorph specific calcium carbonate formation with de novo protein templates

Davila-Hernandez,

Jin,

Pyles

et al. 2023

Nat Commun

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Biomolecules modulate inorganic crystallization to generate hierarchically structured biominerals, but the atomic structure of the organic-inorganic interfaces that regulate mineralization remain largely unknown. We hypothesized that heterogeneous nucleation of calcium carbonate could be achieved by a structured flat molecular template that pre-organizes calcium ions on its surface. To test this hypothesis, we design helical repeat proteins (DHRs) displaying regularly spaced carboxylate arrays on their surfaces and find that both protein monomers and protein-Ca2+ supramolecular assemblies directly nucleate nano-calcite with non-natural {110} or {202} faces while vaterite, which forms first in the absence of the proteins, is bypassed. These protein-stabilized nanocrystals then assemble by oriented attachment into calcite mesocrystals. We find further that nanocrystal size and polymorph can be tuned by varying the length and surface chemistry of the designed protein templates. Thus, bio-mineralization can be programmed using de novo protein design, providing a route to next-generation hybrid materials.

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Formation, Chemical Evolution, and Solidification of the Calcium Carbonate Dense Liquid Phase

Cited by 4 publications

References 24 publications

Molecular simulation approaches to study crystal nucleation from solutions: Theoretical considerations and computational challenges

Molecular simulation approaches to study crystal nucleation from solutions: Theoretical considerations and computational challenges

Theoretical and computational approaches to study crystal nucleation from solution

Directing polymorph specific calcium carbonate formation with de novo protein templates

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