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Title: Copolymer Brush Particle Hybrid Materials with “Recall-and-Repair” Capability

Abstract

The effect of sequence structure on the self-healing and shape-memory properties of copolymer-tethered brush particle films was investigated and compared to linear copolymer analogs. Poly(nbutyl acrylate-co-methyl methacrylate), P(BA-co-MMA), and linear and brush analogs with controlled gradient and statistical sequence were synthesized by atom transfer radical polymerization (ATRP). The effect of sequence on self-healing in BA/MMA copolymer brush particle hybrids followed similar trends as for linear analogs. Most rapid restoration of mechanical properties was found for statistical copolymer sequence; an increase of the high Tg (MMA) component provided a path to raise the material’s modulus while retaining self-heal ability. Creep testing revealed profound differences between linear and brush systems. While linear copolymers featured substantial viscous deformation when exposed to constant stress in the linear regime, brush analogs displayed minimal permanent deformation and featured shape restoration. The reduction of flow was interpreted to be a consequence of slow cooperative relaxation due to the complex microstructure of brush particle hybrids in which long-range motions are constrained through entanglements and slow-diffusing particle cores. The rubbery-like response imparts BA/ MMA copolymer brush material systems concurrent “shape-memory” and “self-heal” capability. This ability to “recall-and-repair” could find application in the design of functional hybrid materials, for example,more » for soft robotics.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Department of Materials Science & Engineering, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, Pennsylvania 15213, United States
  2. Department of Chemistry, Carnegie Mellon University, 4400 Fifth Avenue, Pittsburgh, Pennsylvania 15213, United States
Publication Date:
Research Org.:
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1995555
Alternate Identifier(s):
OSTI ID: 1999507
Grant/Contract Number:  
SC0018784; CMMI-1663305; DMR 2202747; DMR 2209587; DMR 1410845
Resource Type:
Published Article
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Name: Chemistry of Materials Journal Volume: 35 Journal Issue: 17; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical structure; Copolymers; Hybrid materials; Polymers; Self healing materials

Citation Formats

Zhao, Yuqi, Wu, Hanshu, Yin, Rongguan, Yu, Chenxi, Matyjaszewski, Krzysztof, and Bockstaller, Michael R. Copolymer Brush Particle Hybrid Materials with “Recall-and-Repair” Capability. United States: N. p., 2023. Web. doi:10.1021/acs.chemmater.3c01234.
Zhao, Yuqi, Wu, Hanshu, Yin, Rongguan, Yu, Chenxi, Matyjaszewski, Krzysztof, & Bockstaller, Michael R. Copolymer Brush Particle Hybrid Materials with “Recall-and-Repair” Capability. United States. https://doi.org/10.1021/acs.chemmater.3c01234
Zhao, Yuqi, Wu, Hanshu, Yin, Rongguan, Yu, Chenxi, Matyjaszewski, Krzysztof, and Bockstaller, Michael R. Thu . "Copolymer Brush Particle Hybrid Materials with “Recall-and-Repair” Capability". United States. https://doi.org/10.1021/acs.chemmater.3c01234.
@article{osti_1995555,
title = {Copolymer Brush Particle Hybrid Materials with “Recall-and-Repair” Capability},
author = {Zhao, Yuqi and Wu, Hanshu and Yin, Rongguan and Yu, Chenxi and Matyjaszewski, Krzysztof and Bockstaller, Michael R.},
abstractNote = {The effect of sequence structure on the self-healing and shape-memory properties of copolymer-tethered brush particle films was investigated and compared to linear copolymer analogs. Poly(nbutyl acrylate-co-methyl methacrylate), P(BA-co-MMA), and linear and brush analogs with controlled gradient and statistical sequence were synthesized by atom transfer radical polymerization (ATRP). The effect of sequence on self-healing in BA/MMA copolymer brush particle hybrids followed similar trends as for linear analogs. Most rapid restoration of mechanical properties was found for statistical copolymer sequence; an increase of the high Tg (MMA) component provided a path to raise the material’s modulus while retaining self-heal ability. Creep testing revealed profound differences between linear and brush systems. While linear copolymers featured substantial viscous deformation when exposed to constant stress in the linear regime, brush analogs displayed minimal permanent deformation and featured shape restoration. The reduction of flow was interpreted to be a consequence of slow cooperative relaxation due to the complex microstructure of brush particle hybrids in which long-range motions are constrained through entanglements and slow-diffusing particle cores. The rubbery-like response imparts BA/ MMA copolymer brush material systems concurrent “shape-memory” and “self-heal” capability. This ability to “recall-and-repair” could find application in the design of functional hybrid materials, for example, for soft robotics.},
doi = {10.1021/acs.chemmater.3c01234},
journal = {Chemistry of Materials},
number = 17,
volume = 35,
place = {United States},
year = {Thu Aug 17 00:00:00 EDT 2023},
month = {Thu Aug 17 00:00:00 EDT 2023}
}

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