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Abstract Investigating the catalytic behavior of the liquid fuels on well‐defined dual sites is crucial in understanding electrocatalytic reactions. Herein, concept holding bidirectional electronegativity dominant d ‐band center regulation on Pt‐Rh dual sites is proposed to tailor the catalytic behaviors toward methanol oxidation reaction (MOR). The Pt‐Rh dual sites are engineered by introducing the low‐electronegativity Ga/Ni and high‐electronegativity W elements in PtRhGaNiW high‐entropy alloy (HEA), which can drive the electron cloud of Pt‐Rh dual sites redispersing over a wide orbit window. The optimized Pt‐Rh dual sites in PtRhGaNiW HEA nanowire achieve a high current density of 5.61 mA cm −2 toward MOR, which is 3.38 and 9.75 times than that of PtRh alloy (1.66 mA cm −2 ) and Pt/C (0.57 mA cm −2 ), as well as remarkably stability and CO ads poisonous resistance. The theoretical calculations further disclose that the redistribution of surface localized electron around Pt‐Rh dual sites can promote direct oxidation of ─OH, and accelerate the CO ads oxidation/removal. This work presents a breakthrough in designing advanced dual site electrocatalysts for complex catalytic reactions.
Lv et al. (2024) studied this question.