Details
| Original language | English |
|---|---|
| Article number | 111565 |
| Journal | Computational materials science |
| Volume | 212 |
| Early online date | 17 Jun 2022 |
| Publication status | Published - Sept 2022 |
Abstract
Conventional molecular simulations of diffusive molecules in amorphous polymers lead to discrepancies in understanding diffusion mechanisms at low temperatures due to the short timescales of the simulations. This work proposes a combined scheme of the autonomous basin climbing (ABC) method accompanied with kinetic Monte Carlo and reactive molecular dynamics (MD) simulations to investigate water molecules’ diffusion pathways in amorphous epoxy resins across a wide range of temperatures. The ABC method, along with a reactive force field, provides an accurate potential energy surface sampling approach to elucidate diffusion mechanisms affected by hydrogen bonding interactions between water molecules and an epoxy network. The simulation framework allows the capture of thermal effects on the diffusion coefficients and offers a predictive simulation tool for predicting diffusion coefficients of water molecules in amorphous polymers. The simulation results show that the activation energy of the diffusion coefficient is in agreement with experimental data. The proposed simulation framework not only estimates kinetic properties of water diffusion in epoxy resins that are consistent with experimental observations, but also provides a predictive tool for studying the diffusion of small molecules in other amorphous polymers.
Keywords
- Autonomous basin climbing, Epoxy resins, Kinetic Monte Carlo, Reactive molecular dynamics, Water diffusion
ASJC Scopus subject areas
- Computer Science(all)
- General Computer Science
- Chemistry(all)
- General Chemistry
- Materials Science(all)
- General Materials Science
- Engineering(all)
- Mechanics of Materials
- Physics and Astronomy(all)
- General Physics and Astronomy
- Mathematics(all)
- Computational Mathematics
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In: Computational materials science, Vol. 212, 111565, 09.2022.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Elucidating atomistic mechanisms underlying water diffusion in amorphous polymers
T2 - An autonomous basin climbing-based simulation method
AU - Bahtiri, Betim
AU - Arash, Behrouz
AU - Rolfes, Raimund
N1 - Funding Information: This work originates from the following research project: “Challenges of industrial application of nanomodified and hybrid material systems in lightweight rotor blade construction” (“HANNAH - Herausforderungen der industriellen Anwendung von nanomodifizierten und hybriden Werkstoffsystemen im Rotorblattleichtbau”), funded by the Federal Ministry for Economic Affairs and Energy, Germany . The authors wish to express their gratitude for the financial support. The authors acknowledge the support of the LUIS scientific computing cluster, Germany, which is funded by Leibniz Universität Hannover, Germany , the Lower Saxony Ministry of Science and Culture (MWK), Germany and the German Research Council (DFG) .
PY - 2022/9
Y1 - 2022/9
N2 - Conventional molecular simulations of diffusive molecules in amorphous polymers lead to discrepancies in understanding diffusion mechanisms at low temperatures due to the short timescales of the simulations. This work proposes a combined scheme of the autonomous basin climbing (ABC) method accompanied with kinetic Monte Carlo and reactive molecular dynamics (MD) simulations to investigate water molecules’ diffusion pathways in amorphous epoxy resins across a wide range of temperatures. The ABC method, along with a reactive force field, provides an accurate potential energy surface sampling approach to elucidate diffusion mechanisms affected by hydrogen bonding interactions between water molecules and an epoxy network. The simulation framework allows the capture of thermal effects on the diffusion coefficients and offers a predictive simulation tool for predicting diffusion coefficients of water molecules in amorphous polymers. The simulation results show that the activation energy of the diffusion coefficient is in agreement with experimental data. The proposed simulation framework not only estimates kinetic properties of water diffusion in epoxy resins that are consistent with experimental observations, but also provides a predictive tool for studying the diffusion of small molecules in other amorphous polymers.
AB - Conventional molecular simulations of diffusive molecules in amorphous polymers lead to discrepancies in understanding diffusion mechanisms at low temperatures due to the short timescales of the simulations. This work proposes a combined scheme of the autonomous basin climbing (ABC) method accompanied with kinetic Monte Carlo and reactive molecular dynamics (MD) simulations to investigate water molecules’ diffusion pathways in amorphous epoxy resins across a wide range of temperatures. The ABC method, along with a reactive force field, provides an accurate potential energy surface sampling approach to elucidate diffusion mechanisms affected by hydrogen bonding interactions between water molecules and an epoxy network. The simulation framework allows the capture of thermal effects on the diffusion coefficients and offers a predictive simulation tool for predicting diffusion coefficients of water molecules in amorphous polymers. The simulation results show that the activation energy of the diffusion coefficient is in agreement with experimental data. The proposed simulation framework not only estimates kinetic properties of water diffusion in epoxy resins that are consistent with experimental observations, but also provides a predictive tool for studying the diffusion of small molecules in other amorphous polymers.
KW - Autonomous basin climbing
KW - Epoxy resins
KW - Kinetic Monte Carlo
KW - Reactive molecular dynamics
KW - Water diffusion
UR - http://www.scopus.com/inward/record.url?scp=85132425322&partnerID=8YFLogxK
U2 - 10.1016/j.commatsci.2022.111565
DO - 10.1016/j.commatsci.2022.111565
M3 - Article
AN - SCOPUS:85132425322
VL - 212
JO - Computational materials science
JF - Computational materials science
SN - 0927-0256
M1 - 111565
ER -