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Title: Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation

Abstract

Supramolecular associations provide a promising route to functional materials with properties such as self-healing, easy recyclability or extraordinary mechanical strength and toughness. The latter benefit especially from the transient character of the formed network, which enables dissipation of energy as well as regeneration of the internal structures. However, recent investigations revealed intrinsic limitations in the achievable mechanical enhancement. Here we present studies of a set of telechelic polymers with hydrogen-bonding chain ends exhibiting an extraordinarily high, almost glass-like, rubbery plateau. This is ascribed to the segregation of the associative ends into clusters and formation of an interfacial layer surrounding these clusters. An approach adopted from the field of polymer nanocomposites provides a quantitative description of the data and reveals the strongly altered mechanical properties of the polymer in the interfacial layer. These results demonstrate how employing phase separating dynamic bonds can lead to the creation of high-performance materials.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  3. Université de Montpellier (France). Laboratoire Charles Coulomb (L2C)
  4. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1809980
Grant/Contract Number:  
AC05-00OR22725; DMR-1904657
Resource Type:
Accepted Manuscript
Journal Name:
ACS Macro Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 2161-1653
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; associating polymer; supramolecular bond; mechanical reinforcement; phase separation; interfacial layer

Citation Formats

Tress, Martin, Ge, Sirui, Xing, Kunyue, Cao, Peng-Fei, Saito, Tomonori, Genix, Anne-Caroline, and Sokolov, Alexei P. Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation. United States: N. p., 2021. Web. doi:10.1021/acsmacrolett.0c00778.
Tress, Martin, Ge, Sirui, Xing, Kunyue, Cao, Peng-Fei, Saito, Tomonori, Genix, Anne-Caroline, & Sokolov, Alexei P. Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation. United States. https://doi.org/10.1021/acsmacrolett.0c00778
Tress, Martin, Ge, Sirui, Xing, Kunyue, Cao, Peng-Fei, Saito, Tomonori, Genix, Anne-Caroline, and Sokolov, Alexei P. Wed . "Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation". United States. https://doi.org/10.1021/acsmacrolett.0c00778. https://www.osti.gov/servlets/purl/1809980.
@article{osti_1809980,
title = {Turning Rubber into a Glass: Mechanical Reinforcement by Microphase Separation},
author = {Tress, Martin and Ge, Sirui and Xing, Kunyue and Cao, Peng-Fei and Saito, Tomonori and Genix, Anne-Caroline and Sokolov, Alexei P.},
abstractNote = {Supramolecular associations provide a promising route to functional materials with properties such as self-healing, easy recyclability or extraordinary mechanical strength and toughness. The latter benefit especially from the transient character of the formed network, which enables dissipation of energy as well as regeneration of the internal structures. However, recent investigations revealed intrinsic limitations in the achievable mechanical enhancement. Here we present studies of a set of telechelic polymers with hydrogen-bonding chain ends exhibiting an extraordinarily high, almost glass-like, rubbery plateau. This is ascribed to the segregation of the associative ends into clusters and formation of an interfacial layer surrounding these clusters. An approach adopted from the field of polymer nanocomposites provides a quantitative description of the data and reveals the strongly altered mechanical properties of the polymer in the interfacial layer. These results demonstrate how employing phase separating dynamic bonds can lead to the creation of high-performance materials.},
doi = {10.1021/acsmacrolett.0c00778},
journal = {ACS Macro Letters},
number = 2,
volume = 10,
place = {United States},
year = {Wed Jan 13 00:00:00 EST 2021},
month = {Wed Jan 13 00:00:00 EST 2021}
}

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