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

Luo, Xiaoling; Liu, Cheng; Wang, Xiaolei; Shao, Qi; Pi, Yecan; Zhu, Ting; Li, Youyong; Huang, Xiaoqing · Nano Lett · 2020

basic_science · Level V

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Abstract

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 Pd<sub>59</sub>Fe<sub>27</sub>Pt<sub>14</sub> NMs own the highest number of polarized spins (μ<sub>b</sub> = 0.85 μB/f.u.), playing an important role on facilitating the adsorption of OH<sub>ads</sub> to promote the oxidation of CO<sub>ads</sub>, as confirmed by theoretical results. Consequently, the optimized Pd<sub>59</sub>Fe<sub>27</sub>Pt<sub>14</sub> NMs exhibit excellent methanol oxidation reaction activity and stability with a mass activity of 1.61 A mg<sub>Pt</sub><sup>-1</sup>, 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.