Abstract

Fabricating highly efficient Pd-based nanocatalysts with a well-defined structure is desired for the commercialization of direct ethanol fuel cell (DEFC). Herein, a series of hierarchical three-dimensional N-doped hollow graphene spheres (NHGS) supported dendritic PdCu alloy catalysts PdxCu(d)-NHGS (x: Cu/Pd theoretical molar ratio of 4, 2, and 1) are assembled by one-pot ascorbic acid reduction-immobilization method. Aiming to maximize the Pd utilization and realize the efficient ethanol electrooxidation, this novel electrocatalyst offers potent activity sites and promotes electron and ion kinetics simultaneously. Characterization indicates that the as-obtained Pd4Cu(d) alloy nanoparticles with average sizes of approximately 55 nm are evenly dispersed on the NHGS supporting materials obtained by using the SiO2 nanospheres template strategy. Three catalysts all exhibit enhanced electrocatalytic activity, of which the Pd4Cu(d)-NHGS shows the highest mass current activity (2683 mA mgPd-1), which is 2.59 times of the commercial Pd/C toward ethanol electrooxidation in alkaline medium. Based on the results, we believed that the Pd4Cu(d)-NHGS could exhibit extensive application prospect in alkaline DEFC.

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