Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.033
Publication date: 22nd December 2022
With a two million ton global production hydrogen peroxide is a valuable product.[1] Yet it is produced via a non-catalytic and energy intensive anthraquinone process rather than via a sustainable electrochemical procedure.
We have shown that Cu-tmpa can produce hydrogen peroxide upon electrochemical reduction of dioxygen at rates of 1.8 x 106 s–1 and in significant amounts providing that no mass transport limitations in O2 occur.[2] When H2O2 starts to accumulate and O2 concentrations drop overreduction of peroxide to water becomes significant.
We have shown that the rate determining step for O2 reduction is binding of dioxygen to Cu(I), in line with studies by the Karlin group,[3] while reduction of H2O2 appears to proceed via Fenton-like chemistry, showing similarities with lytic polysaccharide monooxygenase chemistry.[4] Despite that strongly oxidative reactive oxygen species are likely to be involved turnover numbers exceed 1000 without any sign of catalyst deactivation.
Detailed mechanistic studies, structure-correlation studies, comparisons with Cu-monooxygenase chemistry, DFT calculations, and experiments to boost the hydrogen peroxide production employing flow cell chemistry and gas diffusion electrodes are in progress.
This work was financially supported by the European Research Council (ERC starting grant 637556 Cu4Energy and ERC proof of concept grant 899535 Cu4peroxide).
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