Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite
Open accessAbstract
We herein show the chiral recognition and separation of aspartic acid (Asp) enantiomers by achiral brushite due to the asymmetries of their dynamical steps in its nonequilibrium states. Growing brushite has a higher adsorption affinity to d-Asp, while l-Asp is predominant on the dissolving brushite surface. Microstructural characterization reveals that chiral selection is mainly attributed to brushite [101] steps, which exhibit two different configurations during crystal growth and dissolution, respectively, with each preferring a distinct enantiomer due to this asymmetry. Because these transition step configurations have different stabilities, they subsequently result in asymmetric adsorption. By varying free energy barriers through solution thermodynamic driving force (i.e., supersaturation), the dominant nonequilibrium intermediate states can be switched and chiral selection regulated. This finding highlights that the dynamic steps can be vital for chiral selection, which may provide a potential pathway for chirality generation through the dynamic nature.
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Very impressive selectivity (around 10% e.e.) was reported for aspartic acid adsorption on brushite under nonequilibrium states but not at saturation.
“Very impressive levels of selectivity (on the range of 10% e.e.) were recently reported for the adsorption of aspartic acid on brushite, a mineral composed of achiral crystals of CaHPO 4 Á 2H 2 O. 283 In this case, selective adsorption was observed under supersaturation and undersaturation conditions (i.e.nonequilibrium states) but not at saturation (equilibrium state).”
From Possible chemical and physical scenarios towards biological homochirality (2022) · cites this paper as [283]
Cites
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Hazen, R. M., & Sholl, D. S. (2003) · Nature Materials · doi:10.1038/nmat879 · Cited by 488 · see citing works
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Possible chemical and physical scenarios towards biological homochirality
Sallembien, Q., Bouteiller, L., Crassous, J., & Raynal, M. (2022) · Chemical Society Reviews · doi:10.1039/d1cs01179k · Cited by 186 · see citing works
- Authors
- Jiang, W., Pan, H., Zhang, Z., Qiu, S. R., Kim, J. D., Xu, X., & Tang, R.
- Affiliations
- Zhejiang University (CN)
- Lawrence Livermore National Laboratory (US)
- Rutgers, The State University of New Jersey (US)
- Corresponding author
- Tang, Ruikang
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-06-15
- Volume
- 139
- Issue
- 25
- Pages
- 8562-8569
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2622885765
- Cited by
- 20
- References
- 3
- Citations by year
- 2026: 1 · 2024: 3 · 2023: 2 · 2022: 1 · 2021: 2 · 2020: 3 · 2019: 3 · 2018: 5
- FWCI
- 1.27
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- Lawrence Livermore National Laboratory (DE-AC52-07NA27344)
- Zhejiang University
- Ministry of Education of the People's Republic of China (2012XZZX005)
- National Natural Science Foundation of China (21571155, 21625105)
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Crystallization and Solubility Studies
- Physical Sciences › Chemistry › Spectroscopy › Analytical Chemistry and Chromatography
- Physical Sciences › Materials Science › Biomaterials › Calcium Carbonate Crystallization and Inhibition
- Keywords
- brushite, aspartic acid, chiral recognition, enantiomer separation, crystal steps, crystal dissolution, supersaturation, activation barrier
- MeSH terms
- Aspartic Acid, Calcium Phosphates, Computer Simulation, Stereoisomerism, Thermodynamics, Microscopy, Atomic Force
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