Probing the reactivity of in situ formed oxygen vacancies of non-noble lead oxides for anodic propylene oxidation
Abstract
Electrochemical oxidation of propylene into value-added products represents a promising strategy for producing commodity chemicals using renewable electricity, thereby aligning with the goals of sustainable chemical manufacturing. While noble metal-based catalysts (e.g., Pd- and Pt-based metal oxides) have been extensively studied for this reaction, the possibility of using non-noble metal-based catalysts and their mechanism remained largely unknown. Herein, we provide the first-ever experimental demonstration of using stable non-noble metal oxide catalysts (i.e., PbO2) for this reaction, and investigate the reaction mechanism of electrochemical propylene oxidation. Electrochemical in situ attenuated total reflection Fourier transform infrared spectroscopy reveals the formation of key surface-bound intermediates during the propylene oxidation process. Moreover, in situ differential electrochemical mass spectrometry confirms the active participation of lattice oxygen in the reaction, suggesting a lattice oxygen-mediated mechanism. These findings shed light on the reaction pathways of non-noble metal catalysts and provide valuable guidance for the rational design of cost-effective and highly selective electrocatalysts for electrochemical alkene oxidation.
 
                




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