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Title: Easy-Processable and Aging-Free All-Polymer Polysiloxane Composites

Abstract

In this work, we report all-polymer polysiloxane composites that overcome the long-standing processing problems of silica-reinforced silicone rubbers. Polystyrene fillers are dispersed with styrene/dimethylsiloxane symmetric diblock and triblock copolymers that control the filler morphology, filler–matrix interactions, and filler–filler interactions. Surprisingly, the composites not only rival the traditional silica-reinforced polysiloxane in mechanical properties of cured materials but also have better processability and stability than the silica-filled compound before curing. Large amplitude oscillatory shear experiments demonstrate that the triblock copolymer addition strongly affects the rheological properties. We hypothesize that the bridges and entangled loops that were formed by the triblock copolymer can connect different PS domains to provide additional reinforcement. The aging effect that originates from PDMS chain adsorption on the filler particle surface is also avoided because of the thermodynamic repulsion between PS and PDMS phases.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [1]
  1. Iowa State Univ., Ames, IA (United States)
  2. Kansas City National Security Campus (KCNSC), Kansas City, MO (United States)
Publication Date:
Research Org.:
Kansas City Nuclear Security Campus (KCNSC), Kansas City, MO (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1826745
Grant/Contract Number:  
NA0002839
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Polymer Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 12; Journal ID: ISSN 2637-6105
Publisher:
ACS Publications
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; polysiloxane composites; block copolymers; polystyrene-b-polydimethylsiloxane; mechanical reinforcement; large amplitude oscillatory shear; transmission electron microscopy

Citation Formats

Shen, Liyang, Wang, Tung-ping, Goyal, Shailja, Lee, Ting-Han, Lin, Fang-Yi, Torres, Sabrina, Robison, Thomas, and Cochran, Eric W. Easy-Processable and Aging-Free All-Polymer Polysiloxane Composites. United States: N. p., 2020. Web. doi:10.1021/acsapm.0c01088.
Shen, Liyang, Wang, Tung-ping, Goyal, Shailja, Lee, Ting-Han, Lin, Fang-Yi, Torres, Sabrina, Robison, Thomas, & Cochran, Eric W. Easy-Processable and Aging-Free All-Polymer Polysiloxane Composites. United States. https://doi.org/10.1021/acsapm.0c01088
Shen, Liyang, Wang, Tung-ping, Goyal, Shailja, Lee, Ting-Han, Lin, Fang-Yi, Torres, Sabrina, Robison, Thomas, and Cochran, Eric W. Thu . "Easy-Processable and Aging-Free All-Polymer Polysiloxane Composites". United States. https://doi.org/10.1021/acsapm.0c01088. https://www.osti.gov/servlets/purl/1826745.
@article{osti_1826745,
title = {Easy-Processable and Aging-Free All-Polymer Polysiloxane Composites},
author = {Shen, Liyang and Wang, Tung-ping and Goyal, Shailja and Lee, Ting-Han and Lin, Fang-Yi and Torres, Sabrina and Robison, Thomas and Cochran, Eric W.},
abstractNote = {In this work, we report all-polymer polysiloxane composites that overcome the long-standing processing problems of silica-reinforced silicone rubbers. Polystyrene fillers are dispersed with styrene/dimethylsiloxane symmetric diblock and triblock copolymers that control the filler morphology, filler–matrix interactions, and filler–filler interactions. Surprisingly, the composites not only rival the traditional silica-reinforced polysiloxane in mechanical properties of cured materials but also have better processability and stability than the silica-filled compound before curing. Large amplitude oscillatory shear experiments demonstrate that the triblock copolymer addition strongly affects the rheological properties. We hypothesize that the bridges and entangled loops that were formed by the triblock copolymer can connect different PS domains to provide additional reinforcement. The aging effect that originates from PDMS chain adsorption on the filler particle surface is also avoided because of the thermodynamic repulsion between PS and PDMS phases.},
doi = {10.1021/acsapm.0c01088},
journal = {ACS Applied Polymer Materials},
number = 12,
volume = 2,
place = {United States},
year = {Thu Nov 19 00:00:00 EST 2020},
month = {Thu Nov 19 00:00:00 EST 2020}
}

Works referenced in this record:

Silicone Elastomer Developments 1967–1977
journal, July 1979

  • Warrick, E. L.; Pierce, O. R.; Polmanteer, K. E.
  • Rubber Chemistry and Technology, Vol. 52, Issue 3
  • DOI: 10.5254/1.3535229

Effect of reinforcing fillers on the rheology of polymer melts
journal, August 1992

  • Aranguren, Mirta I.; Mora, Elsi; DeGroot, Jon V.
  • Journal of Rheology, Vol. 36, Issue 6
  • DOI: 10.1122/1.550306

Block copolymers of polystyrene and poly(dimethyl siloxane). I. Synthesis and characterization
journal, January 1980

  • Bajaj, P.; Varshney, S. K.; Misra, A.
  • Journal of Polymer Science: Polymer Chemistry Edition, Vol. 18, Issue 1
  • DOI: 10.1002/pol.1980.170180128

Large amplitude oscillatory shear behavior of PEO-PPO-PEO triblock copolymer solutions
journal, August 2005


Bound rubber and “crepe hardening” in silicone rubber
journal, December 1977


Characterization of chain binding to filler in silicone-silica systems
journal, August 1985


Elastomer reinforcement from a glassy polymer polymerized in situ
journal, October 1988


A review of nonlinear oscillatory shear tests: Analysis and application of large amplitude oscillatory shear (LAOS)
journal, December 2011


Interpenetrating polymer networks derived from silylated soybean oil and polydimethylsiloxane
journal, May 2013

  • Dewasthale, Sudhanwa; Shi, Xiangke; Hablot, Elodie
  • Journal of Applied Polymer Science, Vol. 130, Issue 4
  • DOI: 10.1002/app.39389

Viscosity–molecular weight relationship for polydimethylsiloxane
journal, May 1966

  • Kataoka, Tadao; Ueda, Shigeyuki
  • Journal of Polymer Science Part B: Polymer Letters, Vol. 4, Issue 5
  • DOI: 10.1002/pol.1966.110040503

Hierarchically Ordered Montmorillonite Block Copolymer Brushes
journal, February 2010

  • Behling, Ross E.; Wolf, Lynn M.; Cochran, Eric W.
  • Macromolecules, Vol. 43, Issue 5
  • DOI: 10.1021/ma902357s

Block copolymer compatibilizers for polystyrene/poly(dimethylsiloxane) blends
journal, January 2002

  • Mari?, M.; Macosko, C. W.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 40, Issue 4
  • DOI: 10.1002/polb.10098

Second‐Order Transition Temperatures and Related Properties of Polystyrene. I. Influence of Molecular Weight
journal, June 1950

  • Fox, Thomas G.; Flory, Paul J.
  • Journal of Applied Physics, Vol. 21, Issue 6
  • DOI: 10.1063/1.1699711

Reinforcement of Silicone Rubber by Particulate Silica
journal, September 1975

  • Boonstra, B. B.; Cochrane, H.; Dánnenberg, E. M.
  • Rubber Chemistry and Technology, Vol. 48, Issue 4
  • DOI: 10.5254/1.3539660

Morphologies of strongly segregated polystyrene-poly(dimethylsiloxane) diblock copolymers
journal, January 1995


Polystyrene- block -Polydimethylsiloxane as a Potential Silica Substitute for Polysiloxane Reinforcement
journal, May 2020


The Influence of Fumed Silica Properties on the Processing, Curing, and Reinforcement Properties of Silicone Rubber
journal, March 1993

  • Cochrane, H.; Lin, C. S.
  • Rubber Chemistry and Technology, Vol. 66, Issue 1
  • DOI: 10.5254/1.3538299

Role of particulate fillers in elastomer reinforcement: a review
journal, June 1979


Elastomers based on α,ω-dihydroxy-polydimethylsiloxane/polystyrene blends: Morphology and mechanical properties
journal, January 2006

  • Dong, Jian; Liu, Zonglin; Cao, Xiaoqun
  • Journal of Applied Polymer Science, Vol. 101, Issue 4
  • DOI: 10.1002/app.23921

Comicellization of Diblock and Triblock Copolymers in Selective Solvents
journal, May 2003

  • Koňák, Čestmír; Helmstedt, Martin
  • Macromolecules, Vol. 36, Issue 12
  • DOI: 10.1021/ma034214n

Melt rheology of organoclay and fumed silica nanocomposites
journal, April 2008


Influence of Polystyrene on PDMS IPNs Blend Membrane Performance
journal, February 2012

  • Pa, Nasrul Fikry Che; Ahmed, Iqbal; Nawawi, Mohd Ghazali Mohd
  • Separation Science and Technology, Vol. 47, Issue 4
  • DOI: 10.1080/01496395.2011.626828

Thermoplastic polydimethylsiloxane with l ‐phenylalanine‐based hydrogen‐bond networks
journal, June 2017

  • Tazawa, Shunsuke; Shimojima, Atsushi; Maeda, Tomoki
  • Journal of Applied Polymer Science, Vol. 135, Issue 24
  • DOI: 10.1002/app.45419

Diblock copolymers as emulsifying agents in polymer blends: Influence of molecular weight, architecture, and chemical composition
journal, July 1996


Preparation and Properties of Polydimethylsiloxane and Its Block Copolymers with Styrene
journal, September 1975

  • Zilliox, J. G.; Roovers, J. E. L.; Bywater, S.
  • Macromolecules, Vol. 8, Issue 5
  • DOI: 10.1021/ma60047a002

Rheology and structure of precipitated silica and poly(dimethyl siloxane) system
journal, March 2004


High χ–Low N Block Polymers: How Far Can We Go?
journal, September 2015


Block Copolymers of Polydimethylsiloxane and Polystyrene
journal, January 1970

  • Saam, John C.; Gordon, David J.; Lindsey, Sarah
  • Macromolecules, Vol. 3, Issue 1
  • DOI: 10.1021/ma60013a001

Rheology of fumed silica/polydimethylsiloxane suspensions
journal, January 2017

  • Ma, Tingting; Yang, Ruiquan; Zheng, Zhong
  • Journal of Rheology, Vol. 61, Issue 2
  • DOI: 10.1122/1.4973974

Aging effects of precipitated silica in poly(dimethylsiloxane)
journal, May 2007

  • Selimovic, Seila; Maynard, Sarah M.; Hu, Yue
  • Journal of Rheology, Vol. 51, Issue 3
  • DOI: 10.1122/1.2714640

The effect of block copolymer architecture on the coalescence and interfacial elasticity in compatibilized polymer blends
journal, May 2005

  • Van Hemelrijck, Ellen; Van Puyvelde, Peter; Macosko, Christopher W.
  • Journal of Rheology, Vol. 49, Issue 3
  • DOI: 10.1122/1.1888625

Structure & strength of silica-PDMS nanocomposites
journal, April 2010


Phase structural formation and oscillation in polystyrene-block-polydimethylsiloxane thin films
journal, January 2012

  • Hsieh, I-Fan; Sun, Hao-Jan; Fu, Qiang
  • Soft Matter, Vol. 8, Issue 30
  • DOI: 10.1039/c2sm25749a

Biobased interpenetrating polymers networks derived from oligomerized soybean oil and polydimethylsiloxane
journal, December 2014

  • Dewasthale, Sudhanwa; Graiver, Daniel; Narayan, Ramani
  • Journal of Applied Polymer Science, Vol. 132, Issue 13
  • DOI: 10.1002/app.41709

Rheological behaviors of fumed silica filled polydimethylsiloxane suspensions
journal, October 2013


Aging Phenomena in Silica-Filled Polydimethylsiloxane
journal, September 1999

  • DeGroot, J. V.; Macosko, C. W.
  • Journal of Colloid and Interface Science, Vol. 217, Issue 1
  • DOI: 10.1006/jcis.1999.6332

Preparation, morphology, and mechanical properties of elastomers based on ?,?-dihydroxy-polydimethylsiloxane/polystyrene blends
journal, January 2004

  • Dong, Jian; Liu, Zonglin; Han, Nianfeng
  • Journal of Applied Polymer Science, Vol. 92, Issue 6
  • DOI: 10.1002/app.20394

Solvent Dependence of the Morphology of Spin-Coated Thin Films of Polydimethylsiloxane-Rich Polystyrene- block -Polydimethylsiloxane Copolymers
journal, June 2012

  • Wadley, Maurice L.; Hsieh, I-Fan; Cavicchi, Kevin A.
  • Macromolecules, Vol. 45, Issue 13
  • DOI: 10.1021/ma300044d

Compounding Fumed Silicas into Polydimethylsiloxane: Bound Rubber and Final Aggregate Size
journal, November 1997

  • Aranguren, Mirta I.; Mora, Elsi; Macosko, Christopher W.
  • Journal of Colloid and Interface Science, Vol. 195, Issue 2
  • DOI: 10.1006/jcis.1997.5143

Preparation, morphology, and mechanical properties of elastomers based on polydimethylsiloxane/ polystyrene blends
journal, April 2009

  • Dong, Jian; Zhang, Naiqiang; Liu, Zonglin
  • Journal of Applied Polymer Science, Vol. 112, Issue 2
  • DOI: 10.1002/app.29486

Reinforcement of elastomeric poly(dimethylsiloxane) by glassy poly(diphenylsiloxane)
journal, January 1990

  • Wang, Shuhong; Mark, J. E.
  • Journal of Materials Science, Vol. 25, Issue 1
  • DOI: 10.1007/BF00544185