Workflow for computational characterization of PDMS cross-linked systems
The aim of this work is to demonstrate a computational workflow for the generation of cross-linkable viscoelastic polymers and the determination of elastic and hyperelastic properties by means of all-atoms classical molecular dynamics simulations, using polydimethylsiloxane (PDMS) as an example. To...
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| Format: | Article |
| Language: | English |
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Frontiers Media S.A.
2023-02-01
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| Series: | Frontiers in Built Environment |
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| Online Access: | https://www.frontiersin.org/articles/10.3389/fbuil.2022.1070045/full |
| _version_ | 1797936237804257280 |
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| author | Steffen Kampmann Alexander Croy Arezoo Dianat Gianaurelio Cuniberti Gianaurelio Cuniberti |
| author_facet | Steffen Kampmann Alexander Croy Arezoo Dianat Gianaurelio Cuniberti Gianaurelio Cuniberti |
| author_sort | Steffen Kampmann |
| collection | DOAJ |
| description | The aim of this work is to demonstrate a computational workflow for the generation of cross-linkable viscoelastic polymers and the determination of elastic and hyperelastic properties by means of all-atoms classical molecular dynamics simulations, using polydimethylsiloxane (PDMS) as an example. To improve the computational efficiency of the workflow, a phenomenological description of the cross-linking process is chosen instead of a quantum mechanical description of the cross-linking mechanism. The structures produced differ in their conversion degree of cross-linking (cdc) of 60, 70, and 80 percent and their quantity ratio between polymer chains and cross-linking units of 2 to 1 and 5 to 1. In order to exclude finite size effects of the molecular systems as much as possible, large systems of about 40,000 atoms are considered. Furthermore, for each possible configuration from the combination of cdc and the ratio of polymer chains to cross-linking units, six structures different from each other are used. Tensile and compression tests are performed to determine mechanical properties. A dependence of stresses in the deformation direction on strain rate is found for strain rates 107, 108, and 109 1/s. As the cdc increases, an increase in the stress values is observed in the tensile tests. To determine the viscoelastic material properties, relaxation tests are performed following the tensile tests. Thereby, the determined relaxed stresses after the tensile test rise with the increase of the cdc. Furthermore, no large stress deviations, .34 MPa maximum, between structures differing by chain to linker ratio are observed with the Ogden model. The computational workflow shows that classical all-atom molecular dynamics simulations can be a suitable method for structure generation and subsequent characterization of elastic and hyperelastic properties of cross-linked polymers. |
| first_indexed | 2024-04-10T18:27:39Z |
| format | Article |
| id | doaj.art-5312b179105f49fab6fdda084ca4ddbb |
| institution | Directory Open Access Journal |
| issn | 2297-3362 |
| language | English |
| last_indexed | 2024-04-10T18:27:39Z |
| publishDate | 2023-02-01 |
| publisher | Frontiers Media S.A. |
| record_format | Article |
| series | Frontiers in Built Environment |
| spelling | doaj.art-5312b179105f49fab6fdda084ca4ddbb2023-02-02T05:20:58ZengFrontiers Media S.A.Frontiers in Built Environment2297-33622023-02-01810.3389/fbuil.2022.10700451070045Workflow for computational characterization of PDMS cross-linked systemsSteffen Kampmann0Alexander Croy1Arezoo Dianat2Gianaurelio Cuniberti3Gianaurelio Cuniberti4Institute for Materials Science and Max Bergmann Center for Biomaterials, TU Dresden, Dresden, GermanyChair of Theoretical Chemistry, Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, GermanyInstitute for Materials Science and Max Bergmann Center for Biomaterials, TU Dresden, Dresden, GermanyInstitute for Materials Science and Max Bergmann Center for Biomaterials, TU Dresden, Dresden, GermanyDresden Center for Computational Materials Science (DCMS), TU Dresden, Dresden, GermanyThe aim of this work is to demonstrate a computational workflow for the generation of cross-linkable viscoelastic polymers and the determination of elastic and hyperelastic properties by means of all-atoms classical molecular dynamics simulations, using polydimethylsiloxane (PDMS) as an example. To improve the computational efficiency of the workflow, a phenomenological description of the cross-linking process is chosen instead of a quantum mechanical description of the cross-linking mechanism. The structures produced differ in their conversion degree of cross-linking (cdc) of 60, 70, and 80 percent and their quantity ratio between polymer chains and cross-linking units of 2 to 1 and 5 to 1. In order to exclude finite size effects of the molecular systems as much as possible, large systems of about 40,000 atoms are considered. Furthermore, for each possible configuration from the combination of cdc and the ratio of polymer chains to cross-linking units, six structures different from each other are used. Tensile and compression tests are performed to determine mechanical properties. A dependence of stresses in the deformation direction on strain rate is found for strain rates 107, 108, and 109 1/s. As the cdc increases, an increase in the stress values is observed in the tensile tests. To determine the viscoelastic material properties, relaxation tests are performed following the tensile tests. Thereby, the determined relaxed stresses after the tensile test rise with the increase of the cdc. Furthermore, no large stress deviations, .34 MPa maximum, between structures differing by chain to linker ratio are observed with the Ogden model. The computational workflow shows that classical all-atom molecular dynamics simulations can be a suitable method for structure generation and subsequent characterization of elastic and hyperelastic properties of cross-linked polymers.https://www.frontiersin.org/articles/10.3389/fbuil.2022.1070045/fullpolymercross-linkingPDMSpolydimethylsiloxanemechanical propertiesrelaxation test |
| spellingShingle | Steffen Kampmann Alexander Croy Arezoo Dianat Gianaurelio Cuniberti Gianaurelio Cuniberti Workflow for computational characterization of PDMS cross-linked systems Frontiers in Built Environment polymer cross-linking PDMS polydimethylsiloxane mechanical properties relaxation test |
| title | Workflow for computational characterization of PDMS cross-linked systems |
| title_full | Workflow for computational characterization of PDMS cross-linked systems |
| title_fullStr | Workflow for computational characterization of PDMS cross-linked systems |
| title_full_unstemmed | Workflow for computational characterization of PDMS cross-linked systems |
| title_short | Workflow for computational characterization of PDMS cross-linked systems |
| title_sort | workflow for computational characterization of pdms cross linked systems |
| topic | polymer cross-linking PDMS polydimethylsiloxane mechanical properties relaxation test |
| url | https://www.frontiersin.org/articles/10.3389/fbuil.2022.1070045/full |
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