Nature Communications · 2024 · 183 citations · 44 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistrySurface ScienceCatalysis At SurfacesCatalyst DeactivationCatalytic MechanismsRedox CatalysisRedox-active MaterialsSurface CatalysisActive SitesCatalyst Active SitesElectrocatalysisElectrocatalystsOrganic Oxidation ReactionsOxidationPulse ElectrolysisSelective Oxidation
Abstract Preventing the deactivation of noble metal-based catalysts due to self-oxidation and poisonous adsorption is a significant challenge in organic electro-oxidation. In this study, we employ a pulsed potential electrolysis strategy for the selective electrocatalytic oxidation of glycerol to glyceric acid over a Pt-based catalyst. In situ Fourier-transform infrared spectroscopy, quasi-in situ X-ray photoelectron spectroscopy, and finite element simulations reveal that the pulsed potential could tailor the catalyst’s oxidation and surface micro-environment. This prevents the overaccumulation of poisoning intermediate species and frees up active sites for the re-adsorption of OH adsorbate and glycerol. The pulsed potential electrolysis strategy results in a higher glyceric acid selectivity (81.8%) than constant-potential electrocatalysis with 0.7 V RHE (37.8%). This work offers an efficient strategy to mitigate the deactivation of noble metal-based electrocatalysts.
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Yifan Yan, Hua Zhou, Simin Xu et al. · Journal of the American Chemical Society · 2023 · 499 citations · Full text