A General Synthetic Method for High-Entropy Alloy Subnanometer Ribbons

过电位 密度泛函理论 成核 合金 结晶 纳米线 化学 电化学 纳米技术 高熵合金 原电池 金属 化学工程 材料科学 电极 物理化学 计算化学 有机化学 工程类
作者
Tao Lü,Mingzi Sun,Yin Zhou,Mingchuan Luo,Fan Lv,Menggang Li,Qinghua Zhang,Lin Gu,Bolong Huang,Shaojun Guo
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:144 (23): 10582-10590 被引量:192
标识
DOI:10.1021/jacs.2c03544
摘要

High-entropy alloys (HEAs) are attracting intensive attention due to their broad compositional tunability and interesting catalytic properties. However, precisely shaping the HEAs into suprathin low-dimensional nanostructures for achieving diverse applications remains an enormous challenge owing to their intrinsic thermodynamic instability. Herein we propose a new and general low-temperature method for incorporating up to eight metallic elements into one single-phase subnanometer ribbon to achieve the thinnest HEA metal materials in the world. We experimentally demonstrate that synthetic processes for suprathin HEA subnanometer ribbons (SNRs) include (1) different metal atom nucleation via galvanic exchange reaction between different metal precursors and Ag nanowire template, (2) co-reduction of different metal precursors on nanowire template, and (3) the removal of the inner Ag core. Density functional theory (DFT) calculations reveal that the crystallization and stabilization of HEA SNRs strongly depend on the "highly dynamic" Ag from the template, and the crystallization levels of HEA subnanometer ribbons are closely correlated with the concentration of Pt and Pd. We demonstrate that the present synthetic method enables the flexible control of components and concentrations in HEAs SNRs for achieving a library of HEA SNRs and also superior electrocatalytic properties. The well-designed HEA SNRs show great improvement in catalyzing the oxygen reduction reaction of fuel cells and also high discharge capacity, low charge overpotential, and excellent durability for Li-O2 batteries. DFT calculations reveal the superior electrochemical performances are attributed to the strong reduction capability from high-concentration reductive elements in HEAs, while the other elements guarantee the site-to-site efficient electron transfer.
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