Crystallization of cross-linked polyethylene by molecular dynamics simulation

Research output: Contribution to journalArticleScientificpeer-review

1 Citation (Scopus)

Abstract

The crystallization of polymers is not, despite its importance in science and engineering, entirely understood due to the challenge of tracking the behavior of individual polymer chains in the crystallizing melt. However, increasing computational resources have brought the crystallization process within reach of molecular simulations, and several groups have published simulations of crystal nucleation and growth in polymers. Yet, these studies have focused on linear polymer chains, and no results have been reported on cross-linked polymers, which are common in everyday applications. Here, we perform molecular dynamics simulations of the homogeneous crystallization of cross-linked polyethylene at high undercooling. Large cross-link densities cause the crystallization to slow down and reduce the final degree of crystallization. As expected, cross-links are rejected from the crystals into the amorphous phase. We observe that at all cross-link densities the intercrystalline amorphous phase is characterized by a single distribution of free segment lengths (amorphous segments with no cross-links). The findings provide a basis for detailed computational studies of semi-crystalline cross-linked polymer systems.

Original languageEnglish
Pages (from-to)80-86
Number of pages7
JournalPolymer
Volume171
DOIs
Publication statusPublished - 8 May 2019
MoE publication typeA1 Journal article-refereed

Fingerprint

Polyethylene
Crystallization
Molecular dynamics
Polyethylenes
Polymers
Computer simulation
Crystals
Undercooling
Nucleation
Crystalline materials

Keywords

  • Cross-linking
  • Crystallization
  • Molecular dynamics
  • Polyethylene

Cite this

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title = "Crystallization of cross-linked polyethylene by molecular dynamics simulation",
abstract = "The crystallization of polymers is not, despite its importance in science and engineering, entirely understood due to the challenge of tracking the behavior of individual polymer chains in the crystallizing melt. However, increasing computational resources have brought the crystallization process within reach of molecular simulations, and several groups have published simulations of crystal nucleation and growth in polymers. Yet, these studies have focused on linear polymer chains, and no results have been reported on cross-linked polymers, which are common in everyday applications. Here, we perform molecular dynamics simulations of the homogeneous crystallization of cross-linked polyethylene at high undercooling. Large cross-link densities cause the crystallization to slow down and reduce the final degree of crystallization. As expected, cross-links are rejected from the crystals into the amorphous phase. We observe that at all cross-link densities the intercrystalline amorphous phase is characterized by a single distribution of free segment lengths (amorphous segments with no cross-links). The findings provide a basis for detailed computational studies of semi-crystalline cross-linked polymer systems.",
keywords = "Cross-linking, Crystallization, Molecular dynamics, Polyethylene",
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Crystallization of cross-linked polyethylene by molecular dynamics simulation. / Paajanen, Antti; Vaari, Jukka; Verho, Tuukka.

In: Polymer, Vol. 171, 08.05.2019, p. 80-86.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - Crystallization of cross-linked polyethylene by molecular dynamics simulation

AU - Paajanen, Antti

AU - Vaari, Jukka

AU - Verho, Tuukka

N1 - Project 107371

PY - 2019/5/8

Y1 - 2019/5/8

N2 - The crystallization of polymers is not, despite its importance in science and engineering, entirely understood due to the challenge of tracking the behavior of individual polymer chains in the crystallizing melt. However, increasing computational resources have brought the crystallization process within reach of molecular simulations, and several groups have published simulations of crystal nucleation and growth in polymers. Yet, these studies have focused on linear polymer chains, and no results have been reported on cross-linked polymers, which are common in everyday applications. Here, we perform molecular dynamics simulations of the homogeneous crystallization of cross-linked polyethylene at high undercooling. Large cross-link densities cause the crystallization to slow down and reduce the final degree of crystallization. As expected, cross-links are rejected from the crystals into the amorphous phase. We observe that at all cross-link densities the intercrystalline amorphous phase is characterized by a single distribution of free segment lengths (amorphous segments with no cross-links). The findings provide a basis for detailed computational studies of semi-crystalline cross-linked polymer systems.

AB - The crystallization of polymers is not, despite its importance in science and engineering, entirely understood due to the challenge of tracking the behavior of individual polymer chains in the crystallizing melt. However, increasing computational resources have brought the crystallization process within reach of molecular simulations, and several groups have published simulations of crystal nucleation and growth in polymers. Yet, these studies have focused on linear polymer chains, and no results have been reported on cross-linked polymers, which are common in everyday applications. Here, we perform molecular dynamics simulations of the homogeneous crystallization of cross-linked polyethylene at high undercooling. Large cross-link densities cause the crystallization to slow down and reduce the final degree of crystallization. As expected, cross-links are rejected from the crystals into the amorphous phase. We observe that at all cross-link densities the intercrystalline amorphous phase is characterized by a single distribution of free segment lengths (amorphous segments with no cross-links). The findings provide a basis for detailed computational studies of semi-crystalline cross-linked polymer systems.

KW - Cross-linking

KW - Crystallization

KW - Molecular dynamics

KW - Polyethylene

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