Mechanically Induced Homochirality in Nucleated Enantioselective Polymerization
Open accessAbstract
Understanding how biological homochirality may have emerged during chemical evolution remains a challenge for origin of life research. In keeping with this goal, we introduce and solve numerically a kinetic rate equation model of nucleated cooperative enantioselective polymerization in closed systems. The microreversible scheme includes (i) solution-phase racemization of the monomers, (ii) linear chain growth by stepwise monomer attachment, in both nucleation and elongation phases, and (iii) annealing or fusion of homochiral chains. Mechanically induced breakage of the longest chains maintains the system out of equilibrium and drives a breakage-fusion recycling mechanism. Spontaneous mirror symmetry breaking can be achieved starting from small initial enantiomeric excesses due to the intrinsic statistical fluctuations about the idealized racemic composition. The subsequent chiral amplification confirms the model's capacity for absolute asymmetric synthesis, without chiral cross-inhibition and without explicit autocatalysis.
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This binary chain fusion mechanism is necessary to achieve SMSB in this simulation from infinitesimal chiral bias (e.e.0 = 5 × 10−11 %).
“This binary chain fusion mechanism is necessary to achieve SMSB in this simulation from infinitesimal chiral bias (e.e. 0 = 5 Â 10 À11 %).”
From Possible chemical and physical scenarios towards biological homochirality (2022) · cites this paper as [578]
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Buhse, T., Cruz, J.-M., Noble-Terán, M. E., Hochberg, D., Ribó, J. M., Crusats, J., & Micheau, J.-C. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00819 · Cited by 189 · see citing works
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Spontaneous mirror symmetry breaking and origin of biological homochirality
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Self-citationThe protometabolic nature of prebiotic chemistry
Nogal, N., Sanz-Sánchez, M., Vela-Gallego, S., Ruiz-Mirazo, K., & de la Escosura, A. (2023) · Chemical Society Reviews · doi:10.1039/d3cs00594a · Cited by 61 · see citing works
- Authors
- Blanco, C., Stich, M., & Hochberg, D.
- Affiliations
- University of California, Santa Barbara (US)
- Aston University (GB)
- Consejo Superior de Investigaciones Científicas (ES)
- Corresponding author
- Hochberg, David
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-01-25
- Volume
- 121
- Issue
- 5
- Pages
- 942-955
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2569862752
- Cited by
- 20
- References
- 7
- Citations by year
- 2025: 3 · 2024: 1 · 2023: 3 · 2022: 4 · 2021: 1 · 2020: 2 · 2019: 4 · 2018: 1 · 2017: 1
- FWCI
- 1.20
- Type
- journal article
- Language
- en
- Open access
- Locations
- The Journal of Physical Chemistry B (publishedVersion)
- PubMed (publishedVersion)
- Aston Publications Explorer (Aston University) (submittedVersion)
- Funders
- Consejo Superior de Investigaciones Científicas (CTQ-2013-47401-C2-2-P)
- Topics
- Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › RNA and protein synthesis mechanisms
- Physical Sciences › Chemistry › Organic Chemistry › Asymmetric Synthesis and Catalysis
- Keywords
- homochirality, origin of life, enantioselective polymerization, nucleation, racemization, mirror symmetry breaking, chiral amplification, absolute asymmetric synthesis, chiral monomers
- MeSH terms
- Stereoisomerism, Thermodynamics, Time Factors, Evolution, Chemical, Polymerization
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