Published June 9, 2023
| Published
Journal Article
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Origin of biological homochirality by crystallization of an RNA precursor on a magnetic surface
Abstract
Homochirality is a signature of life on Earth, yet its origins remain an unsolved puzzle. Achieving homochirality is essential for a high-yielding prebiotic network capable of producing functional polymers like RNA and peptides on a persistent basis. Because of the chiral-induced spin selectivity effect, which established a strong coupling between electron spin and molecular chirality, magnetic surfaces can act as chiral agents and be templates for the enantioselective crystallization of chiral molecules. Here, we studied the spin-selective crystallization of racemic ribo-aminooxazoline (RAO), an RNA precursor, on magnetite (Fe3O4) surfaces, achieving an unprecedented enantiomeric excess (ee) of about 60%. Following the initial enrichment, we then obtained homochiral (100% ee) crystals of RAO after a subsequent crystallization. Our results demonstrate a prebiotically plausible way of achieving system-level homochirality from completely racemic starting materials, in a shallow-lake environment on early Earth where sedimentary magnetite deposits are expected to be common.
Copyright and License
© 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).
Acknowledgement
We thank O. Ben Dor, D. Bhowmick, D. Blackmond, R. Fu, S. Mojzsis, R. Naaman, and J. Szostak for helpful discussions, suggestions, and feedback. We thank V. Loi for the AFM measurements. We acknowledge the Center for Macromolecular Interactions at Harvard Medical School for the use of the CD spectrometer and K. L. Arnett for assistance. We acknowledge the Center for Nanoscale Systems (CNS) and the National Science Foundation’s (NSF) National Nanotechnology Coordinated Infrastructure (NNCI) for the use of the Sharon EE-3 E-Beam Evaporator. We acknowledge the Laukien-Purcell Instrumentation Center for the use of the NMR facility and D. Cui for the assistance. We acknowledge Harvard X-ray Laboratory supported by the Major Research Instrumentation (MRI) Program of the NSF under award number 2216066 and S.-L. Zheng for help with the x-ray data collection and structure determination. We also acknowledge other members of the Simons Collaboration on the Origins of Life and the Harvard Origins of Life Initiative for fruitful discussions that shaped the ideas behind this work.
Funding
This work was supported by a grant from the Simons Foundation (290360) to D.D.S. The Harvard X-ray Laboratory is supported by the Major Research Instrumentation (MRI) Program of the NSF under award number 2216066.
Supplemental Material
Movie S1 (ZIP)
Data S1 to S3 (ZIP)
Files
sciadv.adg8274.pdf
Additional details
- PMCID
- PMC10246896
- PMID
- 37285423
- Simons Foundation
- 290360
- National Science Foundation
- 2216066
- Accepted
-
2023-05-03
- Available
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2023-06-07Published online
- Caltech groups
- Division of Geological and Planetary Sciences (GPS)
- Publication Status
- Published