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Title: Thermal transport in semicrystalline polyethylene by molecular dynamics simulation

Abstract

Recent research has highlighted the potential to achieve high-thermal-conductivity polymers by aligning their molecular chains. Combined with other merits, such as low-cost, corrosion resistance, and light weight, such polymers are attractive for heat transfer applications. Due to their quasi-one-dimensional structural nature, the understanding on the thermal transport in those ultra-drawn semicrystalline polymer fibers or films is still lacking. Here, we built the ideal repeating units of semicrystalline polyethylene and studied their dependence of thermal conductivity on different crystallinity and interlamellar topology using the molecular dynamics simulations. We found that the conventional models, such as the Choy-Young's model, the series model, and Takayanagi's model, cannot accurately predict the thermal conductivity of the quasi-one-dimensional semicrystalline polyethylene. A modified Takayanagi's model was proposed to explain the dependence of thermal conductivity on the bridge number at intermediate and high crystallinity. We also analyzed the heat transfer pathways and demonstrated the substantial role of interlamellar bridges in the thermal transport in the semicrystalline polyethylene. Lastly, our work could contribute to the understanding of the structure–property relationship in semicrystalline polymers and shed some light on the development of plastic heat sinks and thermal management in flexible electronics.

Authors:
 [1];  [2];  [3];  [4];  [5]; ORCiD logo [2]
  1. Tongji University, Shanghai (China); North Carolina State Univ., Raleigh, NC (United States)
  2. North Carolina State Univ., Raleigh, NC (United States)
  3. Huazhong University of Science and Technology, Wuhan (China)
  4. Tongji University, Shanghai (China)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1511161
Alternate Identifier(s):
OSTI ID: 1415667
Grant/Contract Number:  
FG02-02ER45977
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 123; Journal Issue: 1; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 42 ENGINEERING

Citation Formats

Lu, Tingyu, Kim, Kyunghoon, Li, Xiaobo, Zhou, Jun, Chen, Gang, and Liu, Jun. Thermal transport in semicrystalline polyethylene by molecular dynamics simulation. United States: N. p., 2018. Web. doi:10.1063/1.5006889.
Lu, Tingyu, Kim, Kyunghoon, Li, Xiaobo, Zhou, Jun, Chen, Gang, & Liu, Jun. Thermal transport in semicrystalline polyethylene by molecular dynamics simulation. United States. doi:10.1063/1.5006889.
Lu, Tingyu, Kim, Kyunghoon, Li, Xiaobo, Zhou, Jun, Chen, Gang, and Liu, Jun. Thu . "Thermal transport in semicrystalline polyethylene by molecular dynamics simulation". United States. doi:10.1063/1.5006889. https://www.osti.gov/servlets/purl/1511161.
@article{osti_1511161,
title = {Thermal transport in semicrystalline polyethylene by molecular dynamics simulation},
author = {Lu, Tingyu and Kim, Kyunghoon and Li, Xiaobo and Zhou, Jun and Chen, Gang and Liu, Jun},
abstractNote = {Recent research has highlighted the potential to achieve high-thermal-conductivity polymers by aligning their molecular chains. Combined with other merits, such as low-cost, corrosion resistance, and light weight, such polymers are attractive for heat transfer applications. Due to their quasi-one-dimensional structural nature, the understanding on the thermal transport in those ultra-drawn semicrystalline polymer fibers or films is still lacking. Here, we built the ideal repeating units of semicrystalline polyethylene and studied their dependence of thermal conductivity on different crystallinity and interlamellar topology using the molecular dynamics simulations. We found that the conventional models, such as the Choy-Young's model, the series model, and Takayanagi's model, cannot accurately predict the thermal conductivity of the quasi-one-dimensional semicrystalline polyethylene. A modified Takayanagi's model was proposed to explain the dependence of thermal conductivity on the bridge number at intermediate and high crystallinity. We also analyzed the heat transfer pathways and demonstrated the substantial role of interlamellar bridges in the thermal transport in the semicrystalline polyethylene. Lastly, our work could contribute to the understanding of the structure–property relationship in semicrystalline polymers and shed some light on the development of plastic heat sinks and thermal management in flexible electronics.},
doi = {10.1063/1.5006889},
journal = {Journal of Applied Physics},
issn = {0021-8979},
number = 1,
volume = 123,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

FIG.  1 FIG. 1: Schematic diagram of semicrystalline structure, which contains two crystalline regions (white regions on both sides), two interphase regions (gray shaded regions), and an amorphous region (intermediate white region). The inter-phase regions and the amorphous region sandwiched in the middle are defined as an interlamellar region. These regions weremore » distinguished according to the density profiles shown in Appendix B. Crystalline stems are denoted by purple slashes, bridges are denoted by green solid lines, loops are denoted by blue dashed lines, and tails are denoted by orange dotted lines.« less

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Works referenced in this record:

The Halpin-Tsai equations: A review
journal, May 1976

  • Affdl, J. C. Halpin; Kardos, J. L.
  • Polymer Engineering and Science, Vol. 16, Issue 5
  • DOI: 10.1002/pen.760160512

Molecular Simulations of the Interlamellar Phase in Polymers:  Effect of Chain Tilt
journal, November 2000

  • Gautam, S.; Balijepalli, S.; Rutledge, G. C.
  • Macromolecules, Vol. 33, Issue 24
  • DOI: 10.1021/ma0012503

An aqueous, polymer-based redox-flow battery using non-corrosive, safe and low-cost materials
journal, October 2015

  • Janoschka, Tobias; Martin, Norbert; Martin, Udo
  • Nature, Vol. 527, Issue 7576, p. 78-81
  • DOI: 10.1038/nature15746

Kapitza conductance of silicon–amorphous polyethylene interfaces by molecular dynamics simulations
journal, March 2009


High and low thermal conductivity of amorphous macromolecules
journal, January 2017


Improving Electrical Conductivity and Thermal Properties of Polymers by the Addition of Carbon Nanotubes as Fillers
journal, April 2007

  • Winey, Karen I.; Kashiwagi, Takashi; Mu, Minfang
  • MRS Bulletin, Vol. 32, Issue 4
  • DOI: 10.1557/mrs2007.234

Temperature-Dependent Elasticity of a Semicrystalline Interphase Composed of Freely Rotating Chains
journal, September 2003

  • in 't Veld, Pieter J.; Rutledge, Gregory C.
  • Macromolecules, Vol. 36, Issue 19
  • DOI: 10.1021/ma0346658

Anisotropy and structure in uniaxially stretched amorphous high polymers: AMORPHOUS HIGH POLYMERS
journal, January 1967

  • Hennig, Jürgen
  • Journal of Polymer Science Part C: Polymer Symposia, Vol. 16, Issue 5
  • DOI: 10.1002/polc.5070160528

Explicit Treatment of Hydrogen Atoms in Thermal Simulations of Polyethylene
journal, May 2009

  • Henry, Asegun; Chen, Gang
  • Nanoscale and Microscale Thermophysical Engineering, Vol. 13, Issue 2
  • DOI: 10.1080/15567260902834707

Mechanical and Structural Characterization of Semicrystalline Polyethylene under Tensile Deformation by Molecular Dynamics Simulations
journal, June 2015


Electrical and thermal conductivity of polymers filled with metal powders
journal, September 2002


Mechanical properties and fine structure of drawn polymers
journal, January 1967

  • Takayanagi, Motowo; Imada, Kiyohisa; Kajiyama, Tisato
  • Journal of Polymer Science Part C: Polymer Symposia, Vol. 15, Issue 1
  • DOI: 10.1002/polc.5070150118

Thermal Conductivity, Heat Capacity, and Elastic Constants of Water-Soluble Polymers and Polymer Blends
journal, January 2016


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Enhanced thermal conductivity of polymer composites filled with hybrid filler
journal, May 2006


Plastic Deformation of Semicrystalline Polyethylene under Extension, Compression, and Shear Using Molecular Dynamics Simulation
journal, March 2014

  • Kim, Jun Mo; Locker, Rebecca; Rutledge, Gregory C.
  • Macromolecules, Vol. 47, Issue 7
  • DOI: 10.1021/ma402297a

Plastic Deformation of Semicrystalline Polyethylene by Molecular Simulation
journal, April 2011

  • Lee, Sanghun; Rutledge, Gregory C.
  • Macromolecules, Vol. 44, Issue 8
  • DOI: 10.1021/ma1026115

Nonequilirium Molecular Dynamics Methods for Lattice heat Conduction Calculations
journal, January 2014


Thermal conductivity of polymers
journal, October 1977


1D-to-3D transition of phonon heat conduction in polyethylene using molecular dynamics simulations
journal, October 2010


An optimized united atom model for simulations of polymethylene melts
journal, July 1995

  • Paul, Wolfgang; Yoon, Do Y.; Smith, Grant D.
  • The Journal of Chemical Physics, Vol. 103, Issue 4
  • DOI: 10.1063/1.469740

Nonequilibrium Molecular Dynamics Calculation of the Thermal Conductivity of Amorphous Polyamide-6,6
journal, October 2007

  • Lussetti, Enrico; Terao, Takamichi; Müller-Plathe, Florian
  • The Journal of Physical Chemistry B, Vol. 111, Issue 39
  • DOI: 10.1021/jp0737956

Kapitza conductance and phonon scattering at grain boundaries by simulation
journal, June 2004

  • Schelling, P. K.; Phillpot, S. R.; Keblinski, P.
  • Journal of Applied Physics, Vol. 95, Issue 11
  • DOI: 10.1063/1.1702100

Thermal Conductivity in the Radial Direction of Deformed Polymer Fibers
journal, May 2016


Decreased Thermal Conductivity of Polyethylene Chain Influenced by Short Chain Branching
journal, October 2017

  • Luo, Danchen; Huang, Congliang; Huang, Zun
  • Journal of Heat Transfer, Vol. 140, Issue 3
  • DOI: 10.1115/1.4038003

Hybrid Nanorod-Polymer Solar Cells
journal, March 2002

  • Huynh, W. U.; Dittmer, Janke J.; Alivisatos, A. Paul
  • Science, Vol. 295, Issue 5564, p. 2425-2427
  • DOI: 10.1126/science.1069156

The interpretation of dynamic mechanical behavior in ultra high modulus polymers
journal, September 1980

  • Gibson, A. G.; Davies, G. R.; Ward, I. M.
  • Polymer Engineering and Science, Vol. 20, Issue 14
  • DOI: 10.1002/pen.760201405

Role of Chain Morphology and Stiffness in Thermal Conductivity of Amorphous Polymers
journal, January 2016


Chain conformation-dependent thermal conductivity of amorphous polymer blends: the impact of inter- and intra-chain interactions
journal, January 2016

  • Wei, Xingfei; Zhang, Teng; Luo, Tengfei
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 47
  • DOI: 10.1039/C6CP06643G

Novel Polyethylene Fibers of Very High Thermal Conductivity Enabled by Amorphous Restructuring
journal, July 2017


Molecular Dynamics Simulation of the Effects of Layer Thickness and Chain Tilt on Tensile Deformation Mechanisms of Semicrystalline Polyethylene
journal, February 2017


Thermal Conduction in a Single Polyethylene Chain Using Molecular Dynamics Simulations
journal, August 2014


The elasticity and strength of paper and other fibrous materials
journal, March 1952


Thermal conductivity of semicrystalline polymers — a model
journal, August 1977


Effects of chemical bonding on heat transport across interfaces
journal, April 2012

  • Losego, Mark D.; Grady, Martha E.; Sottos, Nancy R.
  • Nature Materials, Vol. 11, Issue 6
  • DOI: 10.1038/nmat3303

Simulation of thermal conductivity and heat transport in solids
journal, February 1999


Bonding-induced thermal conductance enhancement at inorganic heterointerfaces using nanomolecular monolayers
journal, November 2012

  • O’Brien, Peter J.; Shenogin, Sergei; Liu, Jianxiun
  • Nature Materials, Vol. 12, Issue 2
  • DOI: 10.1038/nmat3465

Polyethylene nanofibres with very high thermal conductivities
journal, March 2010

  • Shen, Sheng; Henry, Asegun; Tong, Jonathan
  • Nature Nanotechnology, Vol. 5, Issue 4
  • DOI: 10.1038/nnano.2010.27

Morphology controls the thermoelectric power factor of a doped semiconducting polymer
journal, June 2017

  • Patel, Shrayesh N.; Glaudell, Anne M.; Peterson, Kelly A.
  • Science Advances, Vol. 3, Issue 6
  • DOI: 10.1126/sciadv.1700434

Tuning the thermal conductivity of polymers with mechanical strains
journal, May 2010


Efficient Tandem Polymer Solar Cells Fabricated by All-Solution Processing
journal, July 2007

  • Kim, Jin Young; Lee, Kwanghee; Coates, Nelson E.
  • Science, Vol. 317, Issue 5835, p. 222-225
  • DOI: 10.1126/science.1141711

On the Morphology of Melt-Crystallized Polyethylene I. Lamellar Profiles
journal, June 1981

  • Bassett, D. C.; Hodge, A. M.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 1768
  • DOI: 10.1098/rspa.1981.0113

Hyperelastic characterization of the interlamellar domain and interphase layer in semicrystalline polyethylene
journal, September 2013

  • Ghazavizadeh, Akbar; Rutledge, Gregory C.; Atai, Ali A.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 51, Issue 23
  • DOI: 10.1002/polb.23384

Thermal Conductivity of High-Modulus Polymer Fibers
journal, June 2013

  • Wang, Xiaojia; Ho, Victor; Segalman, Rachel A.
  • Macromolecules, Vol. 46, Issue 12, p. 4937-4943
  • DOI: 10.1021/ma400612y

Thermal Conductance in Cross-linked Polymers: Effects of Non-Bonding Interactions
journal, April 2017

  • Rashidi, Vahid; Coyle, Eleanor J.; Sebeck, Katherine
  • The Journal of Physical Chemistry B, Vol. 121, Issue 17
  • DOI: 10.1021/acs.jpcb.7b01377

Temperature-Dependent Thermal and Elastic Properties of the Interlamellar Phase of Semicrystalline Polyethylene by Molecular Simulation
journal, January 2006

  • in ‘t Veld, Pieter J.; Hütter, Markus; Rutledge, Gregory C.
  • Macromolecules, Vol. 39, Issue 1
  • DOI: 10.1021/ma0518961

VMD: Visual molecular dynamics
journal, February 1996


    Works referencing / citing this record:

    Chain length effect on thermal transport in amorphous polymers and a structure–thermal conductivity relation
    journal, January 2019

    • Wei, Xingfei; Luo, Tengfei
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 28
    • DOI: 10.1039/c9cp02397f