DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Flat-On Secondary Crystals as Effective Blocks To Reduce Ionic Conduction Loss in Polysulfone/Poly(vinylidene fluoride) Multilayer Dielectric Films

Abstract

Recently, poly(vinylidene fluoride) (PVDF)-based multilayer films have demonstrated good potential as high energy density, high temperature, and low loss polymer dielectrics for advanced electrical and power applications. However, impurity ion conduction in the PVDF layers can cause significant dielectric loss at high temperatures. In this study, we discovered a facile melt-recrystallization method to suppress ionic conduction loss in polysulfone (PSF)/PVDF 50/50 (v/v) 33-layer films. By use of combined differential scanning calorimetry, broadband dielectric spectroscopy, and simultaneous small-angle X-ray scattering/wide-angle X-ray diffraction techniques, the underlying mechanism for the suppression of ionic conduction was unraveled. Basically, the growth and hierarchical organization of primary and secondary PVDF crystals confined in 400 nm layers played an important role. When the cooling rate during melt-recrystallization was high (e.g., ≥ 500 °C/min), small and poorly oriented secondary crystals between orderly stacked edge-on primary crystals allowed free transport of impurity ions in PVDF layers. At low to moderate cooling rates (i.e., <100 °C/min), growth of flat-on secondary crystals between the edge-on primary crystalline lamellae blocked the transport of impurity ions, suppressing the dielectric loss from ionic conduction. On the basis of this paper, we propose a modified multilayer coextrusion method with controlled cooling rates to achieve flat-onmore » secondary crystals for the reduction of high temperature dielectric loss in PVDF-based multilayer dielectric films.« less

Authors:
 [1];  [1];  [2];  [2];  [1];  [3];  [3];  [1]; ORCiD logo [1]
  1. Case Western Reserve Univ., Cleveland, OH (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. PolymerPlus, LLC, Valley View, OH (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1462415
Report Number(s):
BNL-207898-2018-JAAM
Journal ID: ISSN 0024-9297
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 51; Journal Issue: 14; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Huang, Huadong, Chen, Xinyue, Li, Ruipeng, Fukuto, Masafumi, Schuele, Donald E., Ponting, Michael, Langhe, Deepak, Baer, Eric, and Zhu, Lei. Flat-On Secondary Crystals as Effective Blocks To Reduce Ionic Conduction Loss in Polysulfone/Poly(vinylidene fluoride) Multilayer Dielectric Films. United States: N. p., 2018. Web. doi:10.1021/acs.macromol.8b01037.
Huang, Huadong, Chen, Xinyue, Li, Ruipeng, Fukuto, Masafumi, Schuele, Donald E., Ponting, Michael, Langhe, Deepak, Baer, Eric, & Zhu, Lei. Flat-On Secondary Crystals as Effective Blocks To Reduce Ionic Conduction Loss in Polysulfone/Poly(vinylidene fluoride) Multilayer Dielectric Films. United States. https://doi.org/10.1021/acs.macromol.8b01037
Huang, Huadong, Chen, Xinyue, Li, Ruipeng, Fukuto, Masafumi, Schuele, Donald E., Ponting, Michael, Langhe, Deepak, Baer, Eric, and Zhu, Lei. Tue . "Flat-On Secondary Crystals as Effective Blocks To Reduce Ionic Conduction Loss in Polysulfone/Poly(vinylidene fluoride) Multilayer Dielectric Films". United States. https://doi.org/10.1021/acs.macromol.8b01037. https://www.osti.gov/servlets/purl/1462415.
@article{osti_1462415,
title = {Flat-On Secondary Crystals as Effective Blocks To Reduce Ionic Conduction Loss in Polysulfone/Poly(vinylidene fluoride) Multilayer Dielectric Films},
author = {Huang, Huadong and Chen, Xinyue and Li, Ruipeng and Fukuto, Masafumi and Schuele, Donald E. and Ponting, Michael and Langhe, Deepak and Baer, Eric and Zhu, Lei},
abstractNote = {Recently, poly(vinylidene fluoride) (PVDF)-based multilayer films have demonstrated good potential as high energy density, high temperature, and low loss polymer dielectrics for advanced electrical and power applications. However, impurity ion conduction in the PVDF layers can cause significant dielectric loss at high temperatures. In this study, we discovered a facile melt-recrystallization method to suppress ionic conduction loss in polysulfone (PSF)/PVDF 50/50 (v/v) 33-layer films. By use of combined differential scanning calorimetry, broadband dielectric spectroscopy, and simultaneous small-angle X-ray scattering/wide-angle X-ray diffraction techniques, the underlying mechanism for the suppression of ionic conduction was unraveled. Basically, the growth and hierarchical organization of primary and secondary PVDF crystals confined in 400 nm layers played an important role. When the cooling rate during melt-recrystallization was high (e.g., ≥ 500 °C/min), small and poorly oriented secondary crystals between orderly stacked edge-on primary crystals allowed free transport of impurity ions in PVDF layers. At low to moderate cooling rates (i.e., <100 °C/min), growth of flat-on secondary crystals between the edge-on primary crystalline lamellae blocked the transport of impurity ions, suppressing the dielectric loss from ionic conduction. On the basis of this paper, we propose a modified multilayer coextrusion method with controlled cooling rates to achieve flat-on secondary crystals for the reduction of high temperature dielectric loss in PVDF-based multilayer dielectric films.},
doi = {10.1021/acs.macromol.8b01037},
journal = {Macromolecules},
number = 14,
volume = 51,
place = {United States},
year = {2018},
month = {7}
}

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

Citation Metrics:
Cited by: 25 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Temperature-scan (A) εr′ and (B) εr″ results for the as-extruded PSF/PVDF 50/50 33L film during first heating, first cooling, and second heating processes between −100 and 180 °C. The heating and cooling rates were 2 °C/min, and the frequency was 1 Hz. Frequency-scan (C) εr′ and (D) εrmore » results at 100 °C for the PSF/PVDF 50/50 33L film before and after melting at 180 °C for 5 min followed by cooling to 100 °C at 5 °C/min.« less

Save / Share:

Works referenced in this record:

Capacitors
journal, January 1998

  • Sarjeant, W. J.; Zirnheld, J.; MacDougall, F. W.
  • IEEE Transactions on Plasma Science, Vol. 26, Issue 5
  • DOI: 10.1109/27.736020

Exploring Strategies for High Dielectric Constant and Low Loss Polymer Dielectrics
journal, October 2014

  • Zhu, Lei
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 21
  • DOI: 10.1021/jz501831q

Advanced polymeric dielectrics for high energy density applications
journal, October 2016


Polymer-Based Dielectrics with High Energy Storage Density
journal, July 2015


50th Anniversary Perspective : Dielectric Phenomena in Polymers and Multilayered Dielectric Films
journal, February 2017


Enhanced breakdown strength of multilayered films fabricated by forced assembly microlayer coextrusion
journal, August 2009


Enhanced dielectric properties due to space charge-induced interfacial polarization in multilayer polymer films
journal, January 2017

  • Chen, Xinyue; Tseng, Jung-Kai; Treufeld, Imre
  • J. Mater. Chem. C, Vol. 5, Issue 39
  • DOI: 10.1039/C7TC03653A

Polymer nanocomposite dielectrics - the role of the interface
journal, August 2005

  • Roy, M.; Nelson, J. K.; MacCrone, R. K.
  • IEEE Transactions on Dielectrics and Electrical Insulation, Vol. 12, Issue 4
  • DOI: 10.1109/TDEI.2005.1511089

The mechanisms leading to the useful electrical properties of polymer nanodielectrics
journal, January 2008

  • Smith, R.; Liang, C.; Landry, M.
  • IEEE Transactions on Dielectrics and Electrical Insulation, Vol. 15, Issue 1
  • DOI: 10.1109/T-DEI.2008.4446750

Ferroelectric Polymers
journal, June 1983


Novel Ferroelectric Polymers for High Energy Density and Low Loss Dielectrics
journal, February 2012


Reduction of Dielectric Hysteresis in Multilayered Films via Nanoconfinement
journal, February 2012

  • Mackey, Matthew; Schuele, Donald E.; Zhu, Lei
  • Macromolecules, Vol. 45, Issue 4
  • DOI: 10.1021/ma202267r

Copolymerization of fluorinated monomers: recent developments and future trends
journal, June 2000


Vinylidene fluoride- and trifluoroethylene-containing fluorinated electroactive copolymers. How does chemistry impact properties?
journal, September 2017


Layer confinement effect on charge migration in polycarbonate/poly(vinylidene fluorid- co -hexafluoropropylene) multilayered films
journal, June 2012

  • Mackey, Matthew; Schuele, Donald E.; Zhu, Lei
  • Journal of Applied Physics, Vol. 111, Issue 11
  • DOI: 10.1063/1.4722348

Reduction of Ionic Conduction Loss in Multilayer Dielectric Films by Immobilizing Impurity Ions in High Glass Transition Temperature Polymer Layers
journal, January 2018

  • Huang, Huadong; Chen, Xinyue; Yin, Kezhen
  • ACS Applied Energy Materials, Vol. 1, Issue 2
  • DOI: 10.1021/acsaem.7b00211

Effects of Impurity Ions on Electrical Properties of Poly(vinylidene fluoride)
journal, November 1982


Reorientational Dynamics of Dipoles in Poly(vinylidene fluoride)/Poly(methyl methacrylate) (PVDF/PMMA) Blends by Dielectric Spectroscopy
journal, May 1997

  • Mijovic, Jovan; Sy, Jo-Wing; Kwei, T. K.
  • Macromolecules, Vol. 30, Issue 10
  • DOI: 10.1021/ma961774w

Confined Crystallization of Polyethylene Oxide in Nanolayer Assemblies
journal, February 2009


Confined Crystallization of PEO in Nanolayered Films Impacting Structure and Oxygen Permeability
journal, September 2009

  • Wang, Haopeng; Keum, Jong K.; Hiltner, Anne
  • Macromolecules, Vol. 42, Issue 18
  • DOI: 10.1021/ma901379f

The effect of confined crystallization on high-density poly(ethylene) lamellar morphology
journal, January 2014


Confined crystallization of PVDF and a PVDF-TFE copolymer in nanolayered films
journal, October 2011

  • Mackey, Matt; Flandin, Lionel; Hiltner, Anne
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 49, Issue 24
  • DOI: 10.1002/polb.22375

Confined crystallization in polymer nanolayered films: A review
journal, February 2012

  • Carr, Joel M.; Langhe, Deepak S.; Ponting, Michael T.
  • Journal of Materials Research, Vol. 27, Issue 10
  • DOI: 10.1557/jmr.2012.17

Annealing effects in poly(vinylidene fluoride) as revealed by specific volume measurements, differential scanning calorimetry, and electron microscopy
journal, November 1973

  • Nakagawa, Koichi; Ishida, Yoichi
  • Journal of Polymer Science Part A-2: Polymer Physics, Vol. 11, Issue 11
  • DOI: 10.1002/pol.1973.180111107

Measurements of Nonlinear Dielectricity in Ferroelectric Polymers
journal, July 1987

  • Furukawa, Takeo; Nakajima, Kenji; Koizumi, Tomoyoshi
  • Japanese Journal of Applied Physics, Vol. 26, Issue Part 1, No. 7
  • DOI: 10.1143/JJAP.26.1039

Understanding Nonlinear Dielectric Properties in a Biaxially Oriented Poly(vinylidene fluoride) Film at Both Low and High Electric Fields
journal, January 2016

  • Li, Yue; Ho, Janet; Wang, Jianchuan
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 1
  • DOI: 10.1021/acsami.5b09368

Quench rates in air, water, and liquid nitrogen, and inference of temperature in volcanic eruption columns
journal, June 2002


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.