Cleavable comonomers enable degradable, recyclable thermoset plastics

Peyton Shieh, Wenxu Zhang, Keith E. L. Husted, Samantha L. Kristufek, Boya Xiong, David J. Lundberg, Jet Lem, David Veysset, Yuchen Sun, Keith A. Nelson, Desiree L. Plata and Jeremiah A. Johnson ()
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Peyton Shieh: Massachusetts Institute of Technology
Wenxu Zhang: Massachusetts Institute of Technology
Keith E. L. Husted: Massachusetts Institute of Technology
Samantha L. Kristufek: Massachusetts Institute of Technology
Boya Xiong: Massachusetts Institute of Technology
David J. Lundberg: Massachusetts Institute of Technology
Jet Lem: Massachusetts Institute of Technology
David Veysset: Massachusetts Institute of Technology
Yuchen Sun: Massachusetts Institute of Technology
Keith A. Nelson: Massachusetts Institute of Technology
Desiree L. Plata: Massachusetts Institute of Technology
Jeremiah A. Johnson: Massachusetts Institute of Technology

Nature, 2020, vol. 583, issue 7817, 542-547

Abstract: Abstract Thermosets—polymeric materials that adopt a permanent shape upon curing—have a key role in the modern plastics and rubber industries, comprising about 20 per cent of polymeric materials manufactured today, with a worldwide annual production of about 65 million tons1,2. The high density of crosslinks that gives thermosets their useful properties (for example, chemical and thermal resistance and tensile strength) comes at the expense of degradability and recyclability. Here, using the industrial thermoset polydicyclopentadiene as a model system, we show that when a small number of cleavable bonds are selectively installed within the strands of thermosets using a comonomer additive in otherwise traditional curing workflows, the resulting materials can display the same mechanical properties as the native material, but they can undergo triggered, mild degradation to yield soluble, recyclable products of controlled size and functionality. By contrast, installation of cleavable crosslinks, even at much higher loadings, does not produce degradable materials. These findings reveal that optimization of the cleavable bond location can be used as a design principle to achieve controlled thermoset degradation. Moreover, we introduce a class of recyclable thermosets poised for rapid deployment.

Date: 2020
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DOI: 10.1038/s41586-020-2495-2

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