Largely boosted methanol electrooxidation using ionic liquid/PdCu aerogels via interface engineering

Abstract

Tuning electrocatalysts via interface engineering is widely adopted as a valid way to manipulate the electrocatalytic activity. Herein, the interface engineering of PdCu aerogels is successfully achieved by the integration of an ionic liquid (IL), which not only accelerates the gelation kinetics but also leads to the modulation of the interface electronic properties, enabling IL functionalized PdCu aerogels (IL/PdCu) as advanced electrocatalysts for the methanol oxidation reaction (MOR) with splendid electrocatalytic activity. Density functional theory (DFT) calculations also demonstrate that IL-involved interface engineering dramatically reduces the chemisorption energy of CO-containing intermediates and thus significantly boosts the MOR performance. Furthermore, direct methanol fuel cells (DMFCs) using an IL/Pd₃Cu₁ anode catalyst exhibit a higher power density than those containing Pd₃Cu₁ and commercial Pd catalysts. This work highlights the superiority of designing advanced electrocatalysts by interface engineering.