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Title: Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films

Abstract

Designing next-generation lightweight pulsed power devices hinges on understanding the factors influencing the energy storage performance of dielectric materials. Polymer dielectric films have a quadratic dependence of energy storage on the voltage breakdown strength and strategies to enhance the breakdown strength are expected to yield a path toward high energy storage densities. Highly stratified lamellar block copolymer (L-BCP) films of model polystyrene-b-polymethylmethacrylate (PS-b-PMMA) exhibited as much as ~50% enhancement in breakdown voltage (E BD), (225 % increase in stored energy density, U~ E BD 2), compared to unordered as-cast L-BCP films. Such an energy density using amorphous polymer is on par with industry-standard semi-crystalline biaxially oriented polypropylene (BOPP), and as such a notable development in the field. This work develops a deeper understanding of the molecular mechanisms of E BD enhancement in L-BCP films, due to combination of interface formation and spatial isolation of the chain ends into segregated zones. We further confirm the role of chain ends in the breakdown process blending a low M n L-BCP with matched M n homopolymers to attain same layer spacing as neat L-BCP of higher M n. E BD shows a significant decrease at low homopolymer fractions due to increased net chainmore » end density within swollen ordered L-BCP domains in wet-brush regime, followed by increased E BD due to layer thickness increase via segregated “interphase layer” formation by excess homopolymers. Notably, E BD of homopolymer swollen L-BCPs is always lower than neat L-BCP of the same domain spacing, due to overall adverse chain ends contribution from homopolymers. These findings provide important selection rules for L-BCPs for designing next-generation flexible electronics with high energy density solid-state BCP film capacitors.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [2];  [3];  [4]; ORCiD logo [5];  [6];  [6];  [7];  [7];  [8]; ORCiD logo [2]
  1. Univ. of Akron, OH (United States)
  2. Univ. of Houston, TX (United States)
  3. UES, Inc., Dayton, OH (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  7. Howard Univ., Washington, DC (United States)
  8. Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
OSTI Identifier:
1656858
Grant/Contract Number:  
AC02-06CH11357; DMR 1901127; DMR 1905996; FA9550-12-1-0306; SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS applied polymer materials
Additional Journal Information:
Journal Volume: ISSN 2637-6105; Journal Issue: 8
Country of Publication:
United States
Language:
English
Subject:
barrier effect; block copolymers; breakdown strength; cold zone annealing-soft shear; dielectric; directed self-assembly; electrostatic capacitors; polymer capacitor

Citation Formats

Samant, Saumil, Basutkar, Monali, Singh, Maninderjeet, Masud, Ali, Grabowski, Christopher A., Kisslinger, Kim, Strzalka, Joseph, Yuan, Guangcui, Satija, Sushil, Apata, Ikeoluwa, Raghavan, Dharmaraj, Durstock, Michael, and Karim, Alamgir. Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films. United States: N. p., 2020. Web. doi:10.1021/acsapm.0c00127.
Samant, Saumil, Basutkar, Monali, Singh, Maninderjeet, Masud, Ali, Grabowski, Christopher A., Kisslinger, Kim, Strzalka, Joseph, Yuan, Guangcui, Satija, Sushil, Apata, Ikeoluwa, Raghavan, Dharmaraj, Durstock, Michael, & Karim, Alamgir. Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films. United States. doi:10.1021/acsapm.0c00127.
Samant, Saumil, Basutkar, Monali, Singh, Maninderjeet, Masud, Ali, Grabowski, Christopher A., Kisslinger, Kim, Strzalka, Joseph, Yuan, Guangcui, Satija, Sushil, Apata, Ikeoluwa, Raghavan, Dharmaraj, Durstock, Michael, and Karim, Alamgir. Tue . "Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films". United States. doi:10.1021/acsapm.0c00127.
@article{osti_1656858,
title = {Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films},
author = {Samant, Saumil and Basutkar, Monali and Singh, Maninderjeet and Masud, Ali and Grabowski, Christopher A. and Kisslinger, Kim and Strzalka, Joseph and Yuan, Guangcui and Satija, Sushil and Apata, Ikeoluwa and Raghavan, Dharmaraj and Durstock, Michael and Karim, Alamgir},
abstractNote = {Designing next-generation lightweight pulsed power devices hinges on understanding the factors influencing the energy storage performance of dielectric materials. Polymer dielectric films have a quadratic dependence of energy storage on the voltage breakdown strength and strategies to enhance the breakdown strength are expected to yield a path toward high energy storage densities. Highly stratified lamellar block copolymer (L-BCP) films of model polystyrene-b-polymethylmethacrylate (PS-b-PMMA) exhibited as much as ~50% enhancement in breakdown voltage (EBD), (225 % increase in stored energy density, U~ EBD2), compared to unordered as-cast L-BCP films. Such an energy density using amorphous polymer is on par with industry-standard semi-crystalline biaxially oriented polypropylene (BOPP), and as such a notable development in the field. This work develops a deeper understanding of the molecular mechanisms of EBD enhancement in L-BCP films, due to combination of interface formation and spatial isolation of the chain ends into segregated zones. We further confirm the role of chain ends in the breakdown process blending a low Mn L-BCP with matched Mn homopolymers to attain same layer spacing as neat L-BCP of higher Mn. EBD shows a significant decrease at low homopolymer fractions due to increased net chain end density within swollen ordered L-BCP domains in wet-brush regime, followed by increased EBD due to layer thickness increase via segregated “interphase layer” formation by excess homopolymers. Notably, EBD of homopolymer swollen L-BCPs is always lower than neat L-BCP of the same domain spacing, due to overall adverse chain ends contribution from homopolymers. These findings provide important selection rules for L-BCPs for designing next-generation flexible electronics with high energy density solid-state BCP film capacitors.},
doi = {10.1021/acsapm.0c00127},
journal = {ACS applied polymer materials},
number = 8,
volume = ISSN 2637-6105,
place = {United States},
year = {2020},
month = {6}
}

Journal Article:
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