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Chiral polymerization: symmetry breaking and entropy production in closed systems
Open accessAbstract
We solve numerically a kinetic model of chiral polymerization in systems closed to matter and energy flow, paying special attention to its ability to amplify the small initial enantiomeric excesses due to the internal and unavoidable statistical fluctuations. The reaction steps are assumed to be reversible, implying a thermodynamic constraint among some of the rate constants. Absolute asymmetric synthesis is achieved in this scheme. The system can persist for long times in quasi-stationary chiral asymmetric states before racemizing. Strong inhibition leads to long-period chiral oscillations in the enantiomeric excesses of the longest homopolymer chains. We also calculate the entropy production σ per unit volume and show that σ increases to a peak value either before or in the vicinity of the chiral symmetry breaking transition.
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Some mechanisms are known for increasing an existing enantiomeric excess, such as self-disproportionation of enantiomers, non-linear effects in asymmetric catalysis, and stereoselective polymerization.
“Some mechanisms are known for increasing an existing e.e., such as the self-disproportionation of enantiomers (SDE), 61 non-linear effects in asymmetric catalysis, 62,63 and stereoselective polymerization.64”
From Possible chemical and physical scenarios towards biological homochirality (2022) · cites this paper as [64]
Polymerization of activated building blocks is discussed as a possible stage for the induction or enhancement of chirality.
“From a different angle, polymerization of activated building blocks is also discussed as a possible stage for the induction/enhancement of chirality, 64 even though prebiotic mechanisms towards these essential-to-life macromolecules remain highly elusive.”
From Possible chemical and physical scenarios towards biological homochirality (2022) · cites this paper as [64]
Starting from an infinitesimal e.e. bias (e.e.0 = 5 × 10−8 %), the Hochberg model shows the emergence of homochiral polymers in an absolute but temporary manner.
“Starting from an infinitesimal e.e. bias (e.e. 0 = 5 Â 10 À8 %), the model shows the emergence of homochiral polymers in an absolute but temporary manner.”
From Possible chemical and physical scenarios towards biological homochirality (2022) · cites this paper as [64]
Citations
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Cited by
Sorted by citations
Prebiotic Systems Chemistry: New Perspectives for the Origins of Life
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Crystalline Architectures as Templates of Relevance to the Origins of Homochirality
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Possible chemical and physical scenarios towards biological homochirality
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Metadata
- Authors
- Blanco, C., & Hochberg, D.
- Affiliations
- Consejo Superior de Investigaciones Científicas (ES)
- Centro de Astrobiología (ES)
- Corresponding author
- Blanco, Celia
- Hochberg, David
- ORCID
- Hochberg, David
- Venue
- Phys. Chem. Chem. Phys.
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2011
- Volume
- 13
- Issue
- 3
- Pages
- 839-849
- ISSN
- 1463-9076 (ISSN-L)
- 1463-9084
- OpenAlex
- W2949813504
- Cited by
- 34
- References
- 4
- Citations by year
- 2026: 2 · 2024: 1 · 2023: 1 · 2022: 5 · 2021: 1 · 2020: 4 · 2019: 2 · 2018: 1 · 2017: 3 · 2016: 2 · 2015: 1 · 2014: 1 · 2013: 1 · 2012: 5
- FWCI
- 1.79
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- Physical Chemistry Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- arXiv (Cornell University)
- Topics
- Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
- Physical Sciences › Physics and Astronomy › Statistical and Nonlinear Physics › Advanced Thermodynamics and Statistical Mechanics
- Physical Sciences › Physics and Astronomy › Statistical and Nonlinear Physics › Complex Systems and Dynamics
- Keywords
- symmetry breaking, entropy production, closed systems, enantiomeric excess, absolute asymmetric synthesis, kinetic model, statistical fluctuations, homopolymer chains, racemization, thermodynamic constraints, kinetic inhibition
- MeSH terms
- Catalysis, Models, Chemical, Polymers, Stereoisomerism, Entropy
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