Mesolytic Cleavage of Homobenzylic Ethers (HBEs) for Programmable End-of-Life Function in Redoxmers

Scientific Achievement

We successfully added an end-of-life function into redoxmers whereby deconstruction is controlled by a redox-triggered mesolytic cleavage of HBE linkages. Using a combined experimental and computational approach, we thoroughly investigated HBE degradation mechanisms, fragmentation pathways, electrochemical properties, and programmable deconstruction of HBE-containing redoxmers from an interface and in bulk solution.

Significance and Impact

Our findings suggest that oxidative cleavage of HBEs facilitate redoxmer-film removal from an interface and bulk deconstruction of redoxmers in solution. Developing redoxmers with programmable deconstruction capabilities improved the resilience of redoxmer-based energy storage materials; this is an important step in development of sustainable energy storage materials for redox flow batteries (RFBs).

Research Detail

  • We synthesized a series of para-substituted HBEs and incorporated them into redox monomers, dimers, and polymers.
  • Experimental and computational results by GC-MS, CV, generation-collection techniques, BE, and DFT revealed mechanistic insights of HBE degradation pathways.
  • We evaluated programmable deconstruction of HBE-containing branched and main-chain redox active polymers at electrode interfaces and in bulk solutions.
  • We presented the vision of end-of-life function in a practical RFB.

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DOI: 10.1039/D1TA10291E

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