Spin Regulation on 2D Pd–Fe–Pt Nanomeshes Promotes Fuel Electrooxidations

Spin engineering provides a powerful strategy for manipulating the interaction between electrons in the d orbital and oxygen-containing adsorbates, while a little endeavor was performed to understand whether such a strategy can make a prosperous enhancement for fuel electrooxidations. Herein, we demonstrate that spin engineering of trimetallic Pd-Fe-Pt nanomeshes (NMs) can achieve superior enhancement for fuel electrooxidations. Magnetization characterizations reveal that Pd₅₉Fe₂₇Pt₁₄ NMs own the highest number of polarized spins (μ_b = 0.85 μB/f.u.), playing an important role on facilitating the adsorption of OH_ads to promote the oxidation of CO_ads, as confirmed by theoretical results. Consequently, the optimized Pd₅₉Fe₂₇Pt₁₄ NMs exhibit excellent methanol oxidation reaction activity and stability with a mass activity of 1.61 A mg_Pt^-1, 2.6-fold and 7.3-fold larger than those of PtRu/C and Pt/C. Such catalysts also present exceptional performances in ethanol oxidation and formic acid oxidation reactions. Our work highlights a new strategy for designing efficient electrocatalysts for fuel electrooxidations and beyond.