Volume 62, Issue 8 e202217941
Research Article

Circular Upcycling of Bottlebrush Thermosets

Dr. Daixuan Zhang

Dr. Daixuan Zhang

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

These authors contributed equally to this work.

Search for more papers by this author
Dr. Foad Vashahi

Dr. Foad Vashahi

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

These authors contributed equally to this work.

Search for more papers by this author
Dr. Erfan Dashtimoghadam

Dr. Erfan Dashtimoghadam

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Dr. Xiaobo Hu

Dr. Xiaobo Hu

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Claire J. Wang

Claire J. Wang

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Jessica Garcia

Jessica Garcia

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Aleksandra V. Bystrova

Aleksandra V. Bystrova

A.N.Nesmeyanov Institute of Organoelement Compounds of Russian Academy of Sciences, Vavilova St. 28, Moscow, 119334 Russian Federation

Search for more papers by this author
Dr. Mohammad Vatankhah-Varnoosfaderani

Dr. Mohammad Vatankhah-Varnoosfaderani

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Prof. Frank A. Leibfarth

Prof. Frank A. Leibfarth

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
Prof. Sergei S. Sheiko

Corresponding Author

Prof. Sergei S. Sheiko

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 USA

Search for more papers by this author
First published: 30 December 2022
Citations: 8

Graphical Abstract

Built-in circularity can be achieved by integrating closed-loop recycling and upcycling in brush-like thermosets with dynamic crosslinks.

Abstract

The inability to re-process thermosets hinders their utility and sustainability. An ideal material should combine closed-loop recycling and upcycling capabilities. This trait is realized in polydimethylsiloxane bottlebrush networks using thermoreversible Diels–Alder cycloadditions to enable both reversible disassembly into a polymer melt and on-demand reconfiguration to an elastomer of either lower or higher stiffness. The crosslink density was tuned by loading the functionalized networks with a controlled fraction of dormant crosslinkers and crosslinker scavengers, such as furan-capped bis-maleimide and anthracene, respectively. The resulting modulus variations precisely followed the stoichiometry of activated furan and maleimide moieties, demonstrating the lack of side reactions during reprocessing. The presented circularity concept is independent from the backbone or side chain chemistry, making it potentially applicable to a wide range of brush-like polymers.

Conflict of interest

The authors declare no conflict of interest

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.