Rational Synthesis of High-Entropy (FeCoNiCuMn)12P5 Microrings and Their Enhanced Hydrogen Evolution Reaction Performance

IF 2.5 4区 化学 Q3 CHEMISTRY, PHYSICAL
Lei Yang, YuXin Wan, Ziyi Zhao, Ziyuan Zhao, Xiaoxian Tian, Jun Yin, Yujue Li, Jiahui Wang, Le Xu, Xueqin Yuan
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Abstract

Designing cost-effective and durable electrocatalysts for the hydrogen evolution reaction (HER) is critical for sustainable energy conversion. Herein, we report the first rational synthesis of high-entropy (FeCoNiCuMn)12P5 microrings on nickel foam via a facile hydrothermal route followed by phosphidation. A gradient control experiment-including (FeCoNiCu)12P5, (FeCoNi)12P5 and Ni12P5 is strategically designed to isolate and verify the entropy effect. Comprehensive characterizations confirm a single phase solid solution with homogeneous elemental distribution and a distinct hollow ring-like morphology. Electrochemical measurements reveal that the high-entropy microrings exhibit the best HER activity, with a low overpotential of 102 mV at 10 mA·cm−2 and a Tafel slope of 61 mV·dec−1, significantly outperforming their lower-entropy counterparts in sequence. Moreover, they demonstrate outstanding long-term durability. The enhanced performance is attributed to the synergistic high‑entropy effect, which modulates the electronic structure and increases the density of accessible active sites. This work not only provides a viable synthetic route toward high‑entropy phosphide microrings but also offers compelling experimental evidence validating the critical role of configurational entropy in boosting HER electrocatalysis.

Graphical Abstract

高熵(FeCoNiCuMn)12P5微环的合理合成及其增强析氢反应性能
为析氢反应(HER)设计经济耐用的电催化剂是实现可持续能量转换的关键。本文首次在泡沫镍上通过简单的水热途径合成了高熵(FeCoNiCuMn)12P5微环,然后进行了磷化反应。设计了梯度控制实验,包括(FeCoNiCu)12P5、(FeCoNi)12P5和Ni12P5,以隔离和验证熵效应。综合表征证实了单相固溶体具有均匀的元素分布和明显的空心环状形态。电化学测量表明,高熵微环表现出最佳的HER活性,在10 mA·cm−2下的过电位为102 mV, Tafel斜率为61 mV·dec−1,显著优于低熵微环。此外,它们具有出色的长期耐用性。增强的性能归因于协同高熵效应,该效应调节了电子结构并增加了可达活性位点的密度。这项工作不仅为高熵磷化物微环的合成提供了可行的途径,而且还提供了令人信服的实验证据,验证了构型熵在促进HER电催化中的关键作用。图形抽象
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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