Revealing the Potential of Ternary Medium-Entropy Alloys as Exceptional Electrocatalysts toward Nitrogen Reduction: An Example of Heusler Alloys

过电位 材料科学 三元运算 电催化剂 催化作用 合金 氨生产 磷化物 电化学 法拉第效率 化学工程 吸附 金属 纳米技术 冶金 物理化学 化学 电极 生物化学 计算机科学 程序设计语言 工程类
作者
Hanqing Yin,Aijun Du
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:14 (13): 15235-15242 被引量:25
标识
DOI:10.1021/acsami.2c00210
摘要

With less energy consumption and environmental pollution, electrochemical ammonia synthesis is regarded as the most promising way to replace the industrial Haber-Bosch process, which greatly contributes to global energy consumption and CO2 emission. At present, the best metal electrocatalyst for N2 fixation is ruthenium although its performance still suffers from a low Faradaic efficiency and a high overpotential. Alloy engineering is a promising way to discover more metal-based electrocatalysts for dinitrogen reduction reaction (N2RR), and almost all reported alloy catalysts so far are binary alloys. In this work, we proposed a large group of ternary alloy electrocatalysts (Heusler alloys) for N2RR and demonstrated their superior catalytic performance. As an example, alloying Ru with Mn and Si led to a reduced Ru-Ru distance on the surface, which facilitates an uncommon horizontal adsorption mode of N2 and results in effective activation of N2 molecules. The theoretical overpotential of N2RR on Ru2MnSi(100-Ru) is only around 0.28 V, which ranks among the best reported results, and the usage of precious Ru is greatly reduced. Meanwhile, the adsorption of N2 on Ru2MnSi(100-Ru) was much stronger than that of protons, and it also took less energy to drive N2RR than the hydrogen evolution reaction (HER), making HER less competitive on this catalyst. Considering the successful synthesis of numerous Heusler alloys including the six members mentioned here, our work provided a wider range of practical and excellent N2RR electrocatalysts in terms of both catalytic performance and economical cost.
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