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Title: Mechanochemical synthesis of glycine oligomers in a virtual rotational diamond anvil cell

Abstract

Mechanochemistry of glycine under compression and shear at room temperature is predicted using quantum-based molecular dynamics (QMD) and a simulation design based on rotational diamond anvil cell (RDAC) experiments. Ensembles of high throughput semiempirical density functional tight binding (DFTB) simulations are used to identify chemical trends and bounds for glycine chemistry during rapid shear under compressive loads of up to 15.6 GPa. Significant chemistry is found to occur during compressive shear above 10 GPa. Recovered products consist of small molecules such as water, structural analogs to glycine, heterocyclic molecules, large oligomers, and polypeptides including the simplest polypeptide glycylglycine at up to 4% mass fraction. The population and size of oligomers generally increases with pressure. A number of oligomeric polypeptide precursors and intermediates are also identified that consist of two or three glycine monomers linked together through C–C, C–N, and/or C–O bridges. Even larger oligomers also form that contain peptide C–N bonds and exhibit branched structures. Many of the product molecules exhibit one or more chiral centers. Our simulations demonstrate that athermal mechanical compressive shearing of glycine is a plausible prebiotic route to forming polypeptides.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
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  1. Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, USA
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1643190
Alternate Identifier(s):
OSTI ID: 1698289
Report Number(s):
LLNL-JRNL-799841
Journal ID: ISSN 2041-6520; CSHCBM
Grant/Contract Number:  
18-LW-036; AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 11 Journal Issue: 30; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Steele, Brad A., Goldman, Nir, Kuo, I-Feng W., and Kroonblawd, Matthew P. Mechanochemical synthesis of glycine oligomers in a virtual rotational diamond anvil cell. United Kingdom: N. p., 2020. Web. doi:10.1039/D0SC00755B.
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Steele, Brad A., Goldman, Nir, Kuo, I-Feng W., & Kroonblawd, Matthew P. Mechanochemical synthesis of glycine oligomers in a virtual rotational diamond anvil cell. United Kingdom. https://doi.org/10.1039/D0SC00755B
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Steele, Brad A., Goldman, Nir, Kuo, I-Feng W., and Kroonblawd, Matthew P. Wed . "Mechanochemical synthesis of glycine oligomers in a virtual rotational diamond anvil cell". United Kingdom. https://doi.org/10.1039/D0SC00755B.
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@article{osti_1643190,
title = {Mechanochemical synthesis of glycine oligomers in a virtual rotational diamond anvil cell},
author = {Steele, Brad A. and Goldman, Nir and Kuo, I-Feng W. and Kroonblawd, Matthew P.},
abstractNote = {Mechanochemistry of glycine under compression and shear at room temperature is predicted using quantum-based molecular dynamics (QMD) and a simulation design based on rotational diamond anvil cell (RDAC) experiments. Ensembles of high throughput semiempirical density functional tight binding (DFTB) simulations are used to identify chemical trends and bounds for glycine chemistry during rapid shear under compressive loads of up to 15.6 GPa. Significant chemistry is found to occur during compressive shear above 10 GPa. Recovered products consist of small molecules such as water, structural analogs to glycine, heterocyclic molecules, large oligomers, and polypeptides including the simplest polypeptide glycylglycine at up to 4% mass fraction. The population and size of oligomers generally increases with pressure. A number of oligomeric polypeptide precursors and intermediates are also identified that consist of two or three glycine monomers linked together through C–C, C–N, and/or C–O bridges. Even larger oligomers also form that contain peptide C–N bonds and exhibit branched structures. Many of the product molecules exhibit one or more chiral centers. Our simulations demonstrate that athermal mechanical compressive shearing of glycine is a plausible prebiotic route to forming polypeptides.},
doi = {10.1039/D0SC00755B},
journal = {Chemical Science},
number = 30,
volume = 11,
place = {United Kingdom},
year = {Wed Aug 05 00:00:00 EDT 2020},
month = {Wed Aug 05 00:00:00 EDT 2020}
}
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https://doi.org/10.1039/D0SC00755B
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