PMID- 36374206
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20221124
IS  - 1520-5207 (Electronic)
IS  - 1520-5207 (Linking)
VI  - 126
IP  - 46
DP  - 2022 Nov 24
TI  - Modeling Method for Semicrystalline Polymers Controlling Aspects of the 
      Morphology at the Molecular Scale for the Study of Mechanical and Physicochemical 
      Properties.
PG  - 9673-9685
LID - 10.1021/acs.jpcb.2c04571 [doi]
AB  - A novel method is presented to build semicrystalline polymer models used in 
      molecular dynamics simulations. The method allows controlling certain aspects of 
      the molecular morphology of the material. It relies on the generation of the 
      polymer sections in the amorphous phase of the semicrystalline structure 
      according to the statistical polymer physics theory proposed by Adhikari and 
      Muthukumar ( J. Chem. Phys.2019, 151, 114905). The amorphous phase is first built 
      based on the method initially developed by Theodorou and Suter ( 
      Macromolecules1985,18 (7), 1467-1478). Then, the amorphous phase is stacked 
      between crystallites, and a connection algorithm proposed by Rigby et al. ( 
      Advanced Composites for Aerospace, Marine, and Land Applications; Springer: Cham, 
      Switzerland, 2014), initially developed to build polymer thermosets, is employed 
      to link the two phases. For a given set of degree of crystallinity, 
      semicrystalline long period, densities of the crystalline and amorphous phases, 
      and polymer molecular weight, the characteristic ratio is used to control the 
      relative fractions of different types of polymer sections in the amorphous phase 
      as well as the distribution of their lengths. There are three types of amorphous 
      polymer sections: the ones that are reentering in the same crystallite called 
      loops, those that are bonding two different crystallites called tie chains, and 
      the chain tails ending in the amorphous region. The higher the imposed 
      characteristic ratio is, the higher the fraction of the tie chains is. The full 
      implementation of the theory is described and then applied to high-density 
      polyethylene (HDPE). Several samples are generated. The obtained structures are 
      characterized. Their elastic coefficients are computed, and high uniaxial 
      deformations are performed. It is shown that the higher the degree of 
      crystallinity, the higher the elastic coefficients. An entanglement analysis 
      shows that the quantity of tie chains is more decisive than the entanglements in 
      acting as stress transmitters to rigidify the structure.
FAU - Belin, Boris
AU  - Belin B
AD  - Institut de Chimie-Physique UMR 8000, Universite Paris Saclay, CNRS, 91405Orsay, 
      France.
AD  - IFP Energies nouvelles, 92852Rueil-Malmaison, France.
AD  - Materials Design SARL, 92120Montrouge, France.
FAU - Yiannourakou, Marianna
AU  - Yiannourakou M
AUID- ORCID: 0000-0001-8467-0957
AD  - Materials Design SARL, 92120Montrouge, France.
FAU - Lachet, Veronique
AU  - Lachet V
AUID- ORCID: 0000-0002-1937-5975
AD  - IFP Energies nouvelles, 92852Rueil-Malmaison, France.
FAU - Rousseau, Bernard
AU  - Rousseau B
AUID- ORCID: 0000-0001-7096-9069
AD  - Institut de Chimie-Physique UMR 8000, Universite Paris Saclay, CNRS, 91405Orsay, 
      France.
LA  - eng
PT  - Journal Article
DEP - 20221114
PL  - United States
TA  - J Phys Chem B
JT  - The journal of physical chemistry. B
JID - 101157530
SB  - IM
EDAT- 2022/11/15 06:00
MHDA- 2022/11/15 06:01
CRDT- 2022/11/14 10:33
PHST- 2022/11/15 06:00 [pubmed]
PHST- 2022/11/15 06:01 [medline]
PHST- 2022/11/14 10:33 [entrez]
AID - 10.1021/acs.jpcb.2c04571 [doi]
PST - ppublish
SO  - J Phys Chem B. 2022 Nov 24;126(46):9673-9685. doi: 10.1021/acs.jpcb.2c04571. Epub 
      2022 Nov 14.