Exceptionally recyclable, extremely tough, vitrimer-like polydimethylsiloxane elastomers via rational network design

Qiyi Chen; Xiao Zhao; Bingrui Li; Alexei P. Sokolov; Ming Tian; Rigoberto C. Advincula; Peng Fei Cao

doi:10.1016/j.matt.2023.05.020

Exceptionally recyclable, extremely tough, vitrimer-like polydimethylsiloxane elastomers via rational network design

Qiyi Chen, Xiao Zhao, Bingrui Li, Alexei P. Sokolov, Ming Tian, Rigoberto C. Advincula, Peng Fei Cao

Research output: Contribution to journal › Article › peer-review

23 Scopus citations

Abstract

Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m³, significantly higher than previously reported PDMS elastomers, excellent chemical resistance, and vitrimer-like rheological behavior. Physical analysis is also performed to provide the accurate estimation of bond-exchange dynamics excluding the often-neglected chain dynamics and to offer insight into the superb performance. We anticipate that such a design principle enables an alternative approach for developing superior recyclable polymer networks.

Original language	English
Pages (from-to)	3378-3393
Number of pages	16
Journal	Matter
Volume	6
Issue number	10
DOIs	https://doi.org/10.1016/j.matt.2023.05.020
State	Published - Oct 4 2023

Funding

Funding: Fundamental Research Funds for the Central Universities ( buctrc202222 ). Work (or part of this work) was done at Oak Ridge National Laboratory, Center for Nanophase Materials Sciences, and Chemical Sciences Division. Funding: Fundamental Research Funds for the Central Universities (buctrc202222). P.-F.C. designed and supervised the research. Initial research directions were identified by Q.C. and P.-F.C. Experimental investigations were conducted by Q.C. with the assistance of X.Z. and B.L. All authors contributed to the writing of the manuscript. The authors declare no competing interests.

Keywords

MAP4: Demonstrate
dynamic study
elastic network
polydimethylsiloxane
recyclability
toughness
vitrimer

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10.1016/j.matt.2023.05.020

Cite this

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title = "Exceptionally recyclable, extremely tough, vitrimer-like polydimethylsiloxane elastomers via rational network design",

abstract = "Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m3, significantly higher than previously reported PDMS elastomers, excellent chemical resistance, and vitrimer-like rheological behavior. Physical analysis is also performed to provide the accurate estimation of bond-exchange dynamics excluding the often-neglected chain dynamics and to offer insight into the superb performance. We anticipate that such a design principle enables an alternative approach for developing superior recyclable polymer networks.",

keywords = "MAP4: Demonstrate, dynamic study, elastic network, polydimethylsiloxane, recyclability, toughness, vitrimer",

author = "Qiyi Chen and Xiao Zhao and Bingrui Li and Sokolov, {Alexei P.} and Ming Tian and Advincula, {Rigoberto C.} and Cao, {Peng Fei}",

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AU - Chen, Qiyi

AU - Zhao, Xiao

AU - Li, Bingrui

AU - Sokolov, Alexei P.

AU - Tian, Ming

AU - Advincula, Rigoberto C.

AU - Cao, Peng Fei

PY - 2023/10/4

Y1 - 2023/10/4

N2 - Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m3, significantly higher than previously reported PDMS elastomers, excellent chemical resistance, and vitrimer-like rheological behavior. Physical analysis is also performed to provide the accurate estimation of bond-exchange dynamics excluding the often-neglected chain dynamics and to offer insight into the superb performance. We anticipate that such a design principle enables an alternative approach for developing superior recyclable polymer networks.

AB - Recently developed elastomers with an adaptable covalent network, e.g., elastic vitrimers, have great potential as sustainable materials, although most of them suffer from limited recyclability and unsatisfied mechanical properties. Here, we report a polydimethylsiloxane (PDMS)-based recyclable elastic network, combining permanent chemical and high-density dynamic physical crosslinks utilizing side-chain reactions, which provides energy dissipation for superb toughness and enables efficient chain rearrangement for excellent recyclability. The optimal elastic network achieves an unprecedented recyclability of 70 cycles, one order of magnitude higher than existing elastic vitrimers, extraordinary toughness of 66 MJ/m3, significantly higher than previously reported PDMS elastomers, excellent chemical resistance, and vitrimer-like rheological behavior. Physical analysis is also performed to provide the accurate estimation of bond-exchange dynamics excluding the often-neglected chain dynamics and to offer insight into the superb performance. We anticipate that such a design principle enables an alternative approach for developing superior recyclable polymer networks.

KW - MAP4: Demonstrate

KW - dynamic study

KW - elastic network

KW - polydimethylsiloxane

KW - recyclability

KW - toughness

KW - vitrimer

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Exceptionally recyclable, extremely tough, vitrimer-like polydimethylsiloxane elastomers via rational network design

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