Work

Advancement of triphos-Ru catalyzed C–O bond disconnections and its challenges

Year: 2026
Type: preprint
Abstract: Cured epoxy resins are crosslinked thermoset materials with applications including carbon-or glass-reinforced composites, but whose extensive C–O and C–N bond networks renders recycling challenging. Previously, our group has reported a Ru-triphos-catalyzed system for the chemical deconstruction of amine-cured epoxy resins, enabling recovery of bisphenol A (BPA) under relatively mild conditions. Subsequent mechanistic studies identified slow catalyst activation and catalyst deactivation as key limitations. Herein, these insights were used to develop improved catalytic systems through pre-catalyst and reaction design. Replacement of the original triphos-Ru-TMM pre-catalyst enabled improved catalytic performance, while ligand design enabled the use of H2, instead of isopropanol, as reductant. Despite these advances, the improved performance observed for model compounds did not translate directly to cured epoxy resins. Reaction optimization revealed pronounced dependencies on substrate concentration, and polymer accessibility, while computational studies suggest changes in catalyst speciation imposed by conformational constraints. Together, these findings demonstrate that the bottlenecks governing epoxy-resin deconstruction can change due to constraints imposed by the polymer matrix. The mechanistic insights obtained herein provide a foundation for the development of next-generation thermoset deconstruction strategies.
Source: ChemRxiv
Language: English
Open Access status: green
OpenAlex ID: W7211868139
Cites: 15
Cited by:
Related to: 10