DOI: 10.1073/pnas.1423898112. Nucleation of metastable aragonite CaCO <sub>3</sub> in seawater

Nucleation of metastable aragonite CaCO 3 in seawater

10.1073/pnas.1423898112

Crossref journal-article

Proceedings of the National Academy of Sciences

Proceedings of the National Academy of Sciences (341)

Abstract

Significance Crystallization from solution is a materials synthesis process common both in nature and in the laboratory. Unlike conventional high-temperature solid-state synthesis, solution-based syntheses often yield metastable phases, contrary to expectations from equilibrium thermodynamics. Using a recently developed ab initio scheme to calculate the surface energy of a critical nucleus in equilibrium with the aqueous environment, we present a framework to compare relative nucleation rates between competing polymorphs as a function of solution chemistry. We apply this approach to demonstrate how seawater chemistry can preferentially bias nucleation toward the metastable aragonite phase of calcium carbonate, rather than the stable phase calcite––which is of great relevance to biomineralization, carbon sequestration, paleogeochemistry, and the vulnerability of marine life to ocean acidification.

Bibliography

Sun, W., Jayaraman, S., Chen, W., Persson, K. A., & Ceder, G. (2015). Nucleation of metastable aragonite CaCO 3 in seawater. Proceedings of the National Academy of Sciences, 112(11), 3199â3204.

Authors 5

Wenhao Sun (first)
Saivenkataraman Jayaraman (additional)
Wei Chen (additional)
Kristin A. Persson (additional)
Gerbrand Ceder (additional)

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Dates

Type	When
Created	10 years, 5 months ago (March 4, 2015, 10:13 p.m.)
Deposited	3 years, 4 months ago (April 13, 2022, 12:32 a.m.)
Indexed	1 day, 5 hours ago (Aug. 31, 2025, 6:10 a.m.)
Issued	10 years, 5 months ago (March 4, 2015)
Published	10 years, 5 months ago (March 4, 2015)
Published Online	10 years, 5 months ago (March 4, 2015)
Published Print	10 years, 5 months ago (March 17, 2015)

Funders 4

U.S. Department of Energy 10.13039/100000015
Region: Americas
gov (National government)
Labels8
1. Energy Department
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Awards1
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U.S. Department of Energy 10.13039/100000015
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U.S. Department of Energy 10.13039/100000015
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BibTeX

@article{Sun_2015, title={Nucleation of metastable aragonite CaCO 3 in seawater}, volume={112}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.1423898112}, DOI={10.1073/pnas.1423898112}, number={11}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Sun, Wenhao and Jayaraman, Saivenkataraman and Chen, Wei and Persson, Kristin A. and Ceder, Gerbrand}, year={2015}, month=mar, pages={3199–3204} }

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