Direct ethanol fuel cells (DEFCs) have been extensively studied as promising energy conversion devices due to their non-toxicity, low corrosivity, and high energy and power densities. However, developing highly active and durable catalysts for the ethanol oxidation reaction (EOR) at the anode remains a significant challenge. Herein, we modulate the intermediate affinity on Pt nanoparticles (NPs) to achieve highly efficient EOR performance through precise optimization of the Pt-CeO2 interface. The well-defined and fully exposed Pt-CeO2 interface was engineered through controlled incorporation of CeO2 nanoclusters within the hierarchical pore structure of nitrogen-doped porous carbon (NPC). The high electrical conductivity and abundant pore structure of NPC not only accelerate the charge transfer rate but also enhance the stability of CeO2 through confinement effects. Importantly, experimental and theoretical analyses reveal that the interaction between CeO2 and Pt NPs strengthens the stability of Pt NPs, modulates the surface charge distribution of Pt, and provides additional adsorbed hydroxyl species (OHads), further boosting the ethanol oxidation capability of Pt. The Pt/CeO2@NPC-300 catalyst not only delivers a maximum mass activity of 1207 mA mgPt-1 and retains 64.7 % of its initial performance after 500 cycles, but also exhibits excellent CO tolerance. This study proposes an innovative catalyst structural design strategy to advance the development of DEFCs and other sustainable energy technologies.
Keywords: Direct ethanol fuel cells; Electronic structure; Ethanol oxidation reaction; Interface engineering; Pt-based catalysts.
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