Synthetic methods that edit soft polymer backbones are critical technologies for tailoring the structures and properties of macromolecules. Developing strategies that leverage underexplored reaction manifolds are vital for accessing new chemical (and functional) space in soft materials. Here, we report a mild electrochemical approach that enables both degradation and functionalization of synthetic polymers. We found that bulk electrolysis (under either homogeneous or heterogeneous conditions) promoted facile, chemoselective chain scission in a variety of olefin-containing materials. Polymer degradation could also be coupled with functionalization (e.g., azidation) to afford new species that could serve as macromonomers.
Metallopolymers are an emerging class of materials with potential utility as semiconductors, catalysts, optical device components, and stimuli responsive networks. While polymer frameworks have been decorated with an array of organometallic moieties, the incorporation of metallocarbenes has been largely overlooked. Here, we report ring-opening metathesis polymerization as a strategy for the synthesis of Fischer carbenecontaining polymers. High degrees of polymerization were observed (>800 repeats), and the isolated materials exhibited exceptional solubility and thermal stability. The tungsten carbene subunits were readily incorporated into block copolymers and could be modified through subsequent transformations. Moreover, the metallocarbene polymers were found to release carbon monoxide upon exposure to light or oxygen, which is unusual for tungsten carbene complexes. These metallocarbenecontaining polymers could represent new platforms for the development of functional materials.
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