Cleavable comonomers enable degradable, recyclable thermoset plastics

• Published in: Nature (London) Vol. 583; no. 7817; pp. 542 - 547
• Main Authors: Shieh, Peyton, Zhang, Wenxu, Husted, Keith E. L., Kristufek, Samantha L., Xiong, Boya, Lundberg, David J., Lem, Jet, Veysset, David, Sun, Yuchen, Nelson, Keith A., Plata, Desiree L., Johnson, Jeremiah A.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 23.07.2020; Nature Publishing Group
• Subjects: 639/301/923/1028; 639/638/455/941; 639/638/455/958; Biodegradation; Chemical properties; Crosslinking; Curing; Degradability; Degradation; Fluorides; Humanities and Social Sciences; Mechanical properties; multidisciplinary; Optimization; Plastics; Polymers; Recyclability; Science; Science (multidisciplinary); Temperature; Tensile strength; Thermal resistance; Thermosetting plastics; Thermosetting resins; United States
• ISSN: 0028-0836; 1476-4687
• DOI: 10.1038/s41586-020-2495-2

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 tons 1 , 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. A method of endowing thermoset plastics with a degree of recyclability and reprocessability by incorporating cleavable chemical linkages in the strands of the polymer, rather than in the crosslinks, is presented.