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Simple, controllable and environmentally friendly synthesis of FeCoNiCuZn-based high-entropy alloy (HEA) catalysts, and their surface dynamics during nitrobenzene hydrogenation

硝基苯 线性扫描伏安法 循环伏安法 介电谱 X射线光电子能谱 苯胺 计时安培法 材料科学 催化作用 伏安法 无机化学 分析化学(期刊) 化学工程 化学 电化学 物理化学 有机化学 工程类 电极
作者
Victor Márquez,Janaína S. Santos,Josephus G. Buijnsters,Supareak Praserthdam,Piyasan Praserthdam
出处
期刊:Electrochimica Acta [Elsevier]
卷期号:410: 139972-139972 被引量:13
标识
DOI:10.1016/j.electacta.2022.139972
摘要

High-entropy alloys (HEAs) have rapidly become one of the hottest research topics in several fields, including materials science, corrosion technology, and catalysis because of their multiple advantages and their potential applications. In this study, using a novel straightforward electroless deposition method, multi-elemental alloys (FeCoNiCuZn) supported on graphite were prepared with controlled metal loading (HEA/g-X; X = 40, 80, 100) without any high temperature post-treatments. These materials were characterized using scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, and showed a composition ranging from 11 at.% to 31 at.% for each metallic element, a total metal loading varying from 1.3 to 5.2 at.% (5.9 to 21.5 wt.%), homogeneous distribution, and an amorphous structure. Electrochemical impedance spectroscopy, cyclic voltammetry, linear sweep voltammetry, and chronoamperometry were used to evaluate the surface dynamics and the effect of the solution pH during the electrochemical hydrogenation of nitrobenzene using the HEA/g-40 material. The nitrobenzene conversion (>9 mmolNB gcat-1 h−1) and aniline production (≈ 4 mmolAN gcat-1 h−1) rates in Na2SO4 solution (at −1.0 V vs. Ag/AgCl) demonstrated a strong dependence on the applied potential. After comparing the results in alkaline medium (KOH), a competitive adsorption of species (nitrobenzene and H2O) was observed, showing a synergistic effect that greatly improved the selectivity of the nitrobenzene hydrogenation to aniline, from 23% in Na2SO4 to an outstanding 94% in KOH at the same applied potential, surpassing the results of a platinum electrode (34% in KOH). These results provide insightful information regarding the nature of the active sites involved in each step of the reaction mechanism, and gives useful means to develop new, tailored multifunctional HEA electrocatalyst materials.
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