<br>高熵金属间化合物 Pt4FeCoCuNi 的有序依赖的析氢和氧还原电催化,Advanced Materials

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高熵金属间化合物 Pt4FeCoCuNi 的有序依赖的析氢和氧还原电催化
Advanced Materials ( IF 27.4 ) Pub Date : 2023-05-10 , DOI: 10.1002/adma.202302067
Yong Wang ₁ , Na Gong ₂ , Hongfei Liu ₂ , Wei Ma ₁ , Kedar Hippalgaonkar _{1,

2} , Zheng Liu ₁ , Yizhong Huang ₁

Affiliation

无序固溶体高熵合金作为坚固的电催化剂引起了广泛的研究关注。相比之下，有序高熵金属间化合物几乎没有被探索过，化学有序程度对催化活性的影响仍然未知。在这项研究中，制备了一系列有序度可调的多组分金属间化合物Pt ₄ FeCoCuNi 纳米颗粒。在单颗粒水平上揭示了多组分纳米粒子从无序结构到有序结构的转变机制，这与选区电子衍射和X射线衍射的宏观分析一致。 Pt ₄ FeCoCuNi 纳米颗粒的电催化性能与其晶体结构和电子结构密切相关。研究发现，增加有序度可以提高电催化性能。高度有序的Pt ₄ FeCoCuNi在酸性氧还原反应（ORR）和碱性析氢反应（HER）方面均实现了最高的质量活性，分别比商业Pt/C高18.9倍和5.6倍。实验还表明，当同时进行 HER 和 ORR 时，该催化剂表现出比部分有序和无序 Pt ₄ FeCoCuNi 以及 Pt/C 更好的长期稳定性。这种依赖于有序的结构-性能关系为催化剂的合理设计提供了见解，并激发了对许多其他多组分金属间合金的探索。

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Ordering-Dependent Hydrogen Evolution and Oxygen Reduction Electrocatalysis of High-Entropy Intermetallic Pt4FeCoCuNi

Disordered solid-solution high-entropy alloys have attracted wide research attention as robust electrocatalysts. In comparison, ordered high-entropy intermetallics have been hardly explored and the effects of the degree of chemical ordering on catalytic activity remain unknown. In this study, a series of multicomponent intermetallic Pt₄FeCoCuNi nanoparticles with tunable ordering degrees is fabricated. The transformation mechanism of the multicomponent nanoparticles from disordered structure into ordered structure is revealed at the single-particle level, and it agrees with macroscopic analysis by selected-area electron diffraction and X-ray diffraction. The electrocatalytic performance of Pt₄FeCoCuNi nanoparticles correlates well with their crystal structure and electronic structure. It is found that increasing the degree of ordering promotes electrocatalytic performance. The highly ordered Pt₄FeCoCuNi achieves the highest mass activities toward both acidic oxygen reduction reaction (ORR) and alkaline hydrogen evolution reaction (HER) which are 18.9-fold and 5.6-fold higher than those of commercial Pt/C, respectively. The experiment also shows that this catalyst demonstrates better long-term stability than both partially ordered and disordered Pt₄FeCoCuNi as well as Pt/C when subject to both HER and ORR. This ordering-dependent structure–property relationship provides insight into the rational design of catalysts and stimulates the exploration of many other multicomponent intermetallic alloys.

更新日期：2023-05-10

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