Pseudo-Jahn-Teller Effect Breaks the pH Dependence in Two-Electron Oxygen Electroreduction.
basic_science · Level V
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- Record sourced from PubMed, PMID 39032092.
- Also identified by DOI 10.1002/adma.202401641.
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Abstract
The hydrogenation of small molecules (like O<sub>2</sub> and CO<sub>2</sub>) often exhibits strong activity dependence on pHs because of discrepant proton donor environments. However, some catalysts can show seldom dependence on two-electron oxygen electroreduction, a sustainable route of O<sub>2</sub> hydrogenation to hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). In this work, a pH-resistant oxygen electroreduction system arising from the pseudo-Jahn-Teller effect is demonstrated. Thorough operando Raman spectra, local environment analyses and density function theory simulations, the lattice distortion of TiO<sub>x</sub>F<sub>y</sub> that introduces the pseudo-Jahn-Teller effect contributing to regulating local pHs at electrode-electrolyte interfaces and the absorption/desorption of key *OOH intermediate is revealed. Consequently, as comparison to 78.6% activity attenuation for common catalyst, the TiO<sub>x</sub>F<sub>y</sub> displays minor activity decay (3.2%) in the pH range of 1-13 with remarkable Faradaic efficiencies (93.4-96.4%) and H<sub>2</sub>O<sub>2</sub> yield rates (595-614 mg cm<sup>-2</sup> h<sup>-1</sup>) in the current densities of 100-1000 mA cm<sup>-2</sup>. Further techno-economics analyses display the H<sub>2</sub>O<sub>2</sub> production cost dependent on pHs, giving the lowest H<sub>2</sub>O<sub>2</sub> price of $0.37 kg<sup>-1</sup>. The present finding is expected to provide an additional dimension to pseudo-Jahn-Teller effect that leverages systems beyond traditional conception.