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    Item type:Publication, Access status: with files ,
    Solvation-controlled accessibility and irreversible finalization of aminoxy intermediates in TEMPO/Benzothiadiazole nonaqueous redox flow batteries
    (American Chemical Society (ACS), 2026-08-19)
    Venter, Hermias
    ;
    Nickel, Ole
    ;
    Meißner, Robert H.
    ;
    Ostermann, Markus
    ;
    Valtiner, Markus
    Understanding how reactive intermediates form and evolve during electrochemical operation is essential for improving the stability of molecular energy-storage systems. Here, we investigate the degradation chemistry of an all-organic nonaqueous redox flow battery based on a nitroxide catholyte and a benzothiadiazole anolyte. By combining electrochemical analysis, full-cell cycling experiments, and molecular dynamics simulations, we reveal how the solvation environment governs both the electrochemical accessibility and the chemical fate of transient reduced intermediates. To rationalize these effects, we introduce a chemically informed framework that decouples electrochemical exposure of parasitic pathways from the probability that such events culminate in irreversible product formation. This minimal model quantitatively captures the relationship between coulombic efficiency and capacity loss across a range of ionic liquid electrolytes, providing a unified description of degradation behavior under realistic operating conditions. Molecular-level analysis further shows that electrolyte-dependent solvation and local coordination environments modulate the stabilization and reactivity of key intermediates, thereby controlling the balance between reversible redox processes and permanent inventory loss. These findings establish a direct link between electrolyte solvation structure and electrochemical degradation pathways, offering a general strategy to diagnose and mitigate failure mechanisms in molecular electrochemical systems. More broadly, the approach provides a conceptual framework for connecting reactive intermediate chemistry with macroscopic device performance in organic energy-storage technologies.
    Publicationtype: Journal Article
      7  5
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    Item type:Publication, Access status: with files ,
    Demonstration of a chemical recycling concept for polybutylene succinate containing waste substrates via coupled enzymatic/electrochemical processes
    (Wiley, 2025-01-31)
    Buchinger, Richard
    ;
    Bischof, Sabrina
    ;
    Nickel, Ole
    ;
    Grassi, Vanessa
    ;
    Antony, Jasmin
    Chemical recycling of polymer waste is a promising strategy to reduce the dependency of chemical industry on fossil resources and reduce the increasing quantities of plastic waste. A common challenge in chemical recycling processes is the costly downstream separation of reaction products. For polybutylene succinate (PBS) no effective recycling concept has been implemented so far. In this work we demonstrate a promising recycling concept for PBS, avoiding costly purification steps. We developed a sequential process, coupling enzymatic hydrolysis of PBS with an electrochemical reaction step. The enzymatic step efficiently hydrolyses PBS in its monomers, succinic acid and 1,4-butanediol. The electrochemical step converts succinic acid into ethene as final product. Ethene is easily separated from the reaction solution as gaseous product, together with hydrogen as secondary product, while 1,4-butanediol remains in the aqueous solution. Both reaction steps operate in aqueous solvent and benign reaction conditions. Furthermore, the influence of electrolyte components on the electrochemical step was unraveled by applying molecular dynamic simulations. The final coupled process achieves a total ethene productivity of 91 μmol/cm2 over a duration of 8 hours, with 1110 μmol/cm2 hydrogen and 77 % regained 1,4-butanediol as valuable secondary products.
    Publicationtype: Journal Article
      10  9