Abstract
Modulating the d-orbital electronic structure of active metals by doping heteroatoms is efficient for the electro-catalysis of methanol oxidation reaction (MOR). However, precise doping hybrid atoms into the lattices of alloy catalysts remains challenging. Herein, the selected doping of electron-rich P atoms at the active site of Pd was achieved by hydrothermal reduction. We found that P atoms prefer to bond Pd atoms, thus tuning the electronic structure of active sites in PdCoP alloy. Consequently, the tailored PdCoP catalyst exhibited remarkable mass activity of 2.13 A mgPd−1 towards MOR, which surpasses most reported Pd-based alloy nanocatalysts. Theoretical calculations revealed that the tailored d-band center of Pd in PdCoP catalyst exhibited moderate adsorption of CO and OH intermediates, thus maximizing the MOR performance. The current work highlights the fabrication of P-doped Pd-based catalysts for realizing high MOR, which can be further extended to other energy-related applications.
Published Version
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