Dual C–H functionalization of polyolefins for covalent adaptable network formation via cooperative electrolysis

Zhou, Yuting [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000287519686); Xu, Zhenchuang [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000193173231); Moore, Jeffrey S. [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000158416269)

doi:10.1038/s44160-025-00876-7

DOE OSTI · 3023205

Dual C–H functionalization of polyolefins for covalent adaptable network formation via cooperative electrolysis

Zhou, Yuting [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000287519686)·Xu, Zhenchuang [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000193173231)·Moore, Jeffrey S. [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000158416269)

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Abstract

The increasing demand for carbon fibre-reinforced polymer composites with polyolefin thermoset matrices will lead to the generation of large volumes of low molecular weight waste oligomers during the fibre recovery process. To address this challenge, we present a cooperative electrolytic dual C–H bond functionalization strategy for the one-step installation of two key functional groups essential for dynamic linkages of these deconstructed oligomers. Through direct competition studies, we reveal the predominance of tertiary allylic C–H activation along the complex, branched oligomer backbone. The resulting difunctionalized oligomers form covalently adaptable networks with exceptional circularity. By establishing a sustainable pathway for upcycling deconstructed oligomers from carbon fibre-reinforced polymer fibre recovery, this strategy introduces thermoset materials derived directly from waste. Here, it advances sustainable manufacturing practices, contributing to a net-zero waste synthetic ecosystem, and highlights the prospects of mediated electrolysis in macromolecular transformations.

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Zhou, Yuting [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000287519686), Xu, Zhenchuang [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000193173231), Moore, Jeffrey S. [University of Illinois at Urbana−Champaign, IL (United States)] (ORCID:0000000158416269). 2025-09-18. Dual C–H functionalization of polyolefins for covalent adaptable network formation via cooperative electrolysis. https://doi.org/10.1038/s44160-025-00876-7

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