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 (μb = 0.85 μB/f.u.), playing an important role on facilitating the adsorption of OHads to promote the oxidation of COads, 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 mgPt-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.