Sub-2 nm Ultrasmall High-Entropy Alloy Nanoparticles for Extremely Superior Electrocatalytic Hydrogen Evolution,Journal of the American Chemical Society

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Sub-2 nm Ultrasmall High-Entropy Alloy Nanoparticles for Extremely Superior Electrocatalytic Hydrogen Evolution
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-09-23 , DOI: 10.1021/jacs.1c07643
Guang Feng ₁ , Fanghua Ning ₁ , Jin Song ₁ , Huaifang Shang ₁ , Kun Zhang ₁ , Zhengping Ding ₂ , Peng Gao ₂ , Wangsheng Chu ₃ , Dingguo Xia _{1,

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Affiliation

The development of sufficiently effective catalysts with extremely superior performance for electrocatalytic hydrogen production still remains a formidable challenge, especially in acidic media. Here, we report ultrasmall high-entropy alloy (us-HEA) nanoparticles (NPs) with the best-level performance for hydrogen evolution reaction (HER). The us-HEA (NiCoFePtRh) NPs show an average diameter of 1.68 nm, which is the smallest size in the reported HEAs. The atomic structure, coordinational structure, and electronic structure of the us-HEAs were comprehensively clarified. The us-HEA/C achieves an ultrahigh mass activity of 28.3 A mg^–1_{noble metals} at −0.05 V (vs the reversible hydrogen electrode, RHE) for HER in 0.5 M H₂SO₄ solution, which is 40.4 and 74.5 times higher than those of the commercial Pt/C and Rh/C catalysts, respectively. Moreover, the us-HEA/C demonstrates an ultrahigh turnover frequency of 30.1 s^–1 at 50 mV overpotential (41.8 times higher than that of the Pt/C catalyst) and excellent stability with no decay after 10 000 cycles. Operando X-ray absorption spectroscopy and theoretical calculations reveal the actual active sites, tunable electronic structures, and a synergistic effect among five elements, which endow significantly enhanced HER activity. This work not only engineers a general and scalable strategy for synthesizing us-HEA NPs and elucidates the complex structural information and catalytic mechanisms of multielement HEA system in depth, but also highlights HEAs as sufficiently advanced catalysts and accelerates the research of HEAs in energy-related applications.

中文翻译：

亚 2 nm 超小型高熵合金纳米粒子，用于极其出色的电催化制氢

开发具有极其优异性能的电催化制氢催化剂仍然是一项艰巨的挑战，尤其是在酸性介质中。在这里，我们报告了具有最佳析氢反应 (HER) 性能的超小型高熵合金 (us-HEA) 纳米粒子 (NPs)。us-HEA (NiCoFePtRh) NPs 的平均直径为 1.68 nm，这是报告的 HEA 中最小的尺寸。全面阐明了us-HEAs的原子结构、配位结构和电子结构。us-HEA/C在 0.5 MH ₂ SO _{4 中的}HER 在 -0.05 V（相对于可逆氢电极，RHE）下实现了 28.3 A mg ^–1_贵金属的超高质量活性溶液，分别是商业 Pt/C 和 Rh/C 催化剂的 40.4 和 74.5 倍。此外，us-HEA/C 展示了 30.1 s ^–1的超高周转频率在 50 mV 过电位下（比 Pt/C 催化剂高 41.8 倍）和优异的稳定性，10 000 次循环后没有衰减。Operando X 射线吸收光谱和理论计算揭示了实际的活性位点、可调电子结构以及五种元素之间的协同效应，这些都显着增强了 HER 活性。这项工作不仅设计了合成 us-HEA NPs 的通用且可扩展的策略，并深入阐明了多元素 HEA 系统的复杂结构信息和催化机制，而且突出了 HEA 作为足够先进的催化剂，并加速了 HEA 在能源相关领域的研究。应用程序。

更新日期：2021-10-20

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