摘要
Against the backdrop of global carbon neutrality target driving the transformation of energy structure, alcohol fuel cells (AFCs) show great application potential; However, the sluggish kinetics of their anodic alcohol oxidation reaction hinders the commercialization of AFCs. Metallene is a novel 2D material with potential application prospect in the field of electrocatalysis. In this paper, Pd 1 Mo 1 W trimetallene has been successfully produced by a one-pot wet-chemical method, which displays a unique two-dimensional curved ultrathin graphene structure. Mo and W atoms were doped into the lattice of Pd atoms to form a Pd 1 Mo 1 W ternary alloy, which resulted in the lattice spacing of Pd being enlarged to 0.229 nm and the d-band center of Pd being reduced by 1.10 eV. Therefore, Pd 1 Mo 1 W trimetallene demonstrated excellent electrocatalytic performance for the oxidation of ethanol and ethylene glycol in alkaline electrolyte. Especially for the ethanol oxidation reaction (EOR), Pd 1 Mo 1 W trimetallene exhibited excellent mass activity (7.55 A mg Pd −1 ) and intrinsic activity (13.5 mA cm −2 ), low apparent activation energy (41.8 kJ mol −1 ), and outstanding CO anti-poisoning ability. According to the nuclear magnetic resonance, in-situ fourier transform infrared reflection spectra, and density-functional theory calculations, it is revealed that the Pd 1 Mo 1 W trimetallene with high surface area formed by Mo-doping reduces the d-band center of the active site, facilitates the adsorption of OH species, and enhances the tolerance of CO-poisoned intermediate, so that EOR can be carried out through C1 and C2 pathways at a lower potential. Compared to the electrocatalytic EOR system, the photocurrent density of Pd 1 Mo 1 W trimetallene under xenon lamp irradiation increased by 1.73 times, which was mainly attributed to the electron resonance effect generated by Mo and W elements to promote the electron transfer to Pd. The excellent electrocatalytic ethanol and ethylene glycol performance of Pd 1 Mo 1 W demonstrates the great application potential of metallene for electrocatalysis.
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