摘要
The increasing availability of active sites and optimizing electronic state of active metals are powerful strategies to rationally fabricate electrocatalysts with both high activity and long-term durability towards ethanol oxidation reaction (EOR). In this study, we fabricate a new catalyst, Pd nanocrystals (NCs) anchored on the embedded nanodiamonds (ND) into nitrogen-doped graphene (NG) aerogel (Pd/ND@NG). As an electrocatalyst for EOR in alkaline conditions, the optimized-Pd/ND@NG-2 achieves improved electrocatalytic activity (with a mass activity of 1338.0 mA mg −1 ) and reinforced poison resistance along with exceptional durability of minimal current decay after stability test, which are markedly surpassing those of commercial Pd/C (685.2 mA mg −1 ). Integrating the electrocatalytic measurements and systematic characterizations underscore the crucial roles of embedded ND into NG in enhancing electrocatalytic behavior of EOR. In brief, the embedded ND into NG observably increases the specific surface area and porosity of the prepared-electrocatalysts, which not only provides abundant channels for the mass/charge transfer but also increases the active sites availability through the high dispersion of small-sized Pd NCs on ND@NG supports. More importantly, the embedded ND into NG creates electron-deficient active Pd, which facilitates the adsorption of electron-rich intermediates (OH ads ) and the desorption of electron-deficient toxic intermediates (CO ads ), thereby boosting its electrocatalytic activity and durability. Additionally, this work provides an effective and practical strategy for assembling graphene aerogel, and offering insights for the development of research and application in electrocatalysis and beyond.
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