Enhancing Oxygen Evolution Reaction Performance in Prussian Blue Analogues: Triple‐Play of Metal Exsolution, Hollow Interiors, and Anionic Regulation

普鲁士蓝 析氧 材料科学 催化作用 分解水 塔菲尔方程 化学工程 纳米颗粒 过电位 金属 纳米技术 化学 光催化 电极 物理化学 冶金 有机化学 工程类 电化学
作者
Shiqi Wang,Wenyi Huo,Hanchen Feng,Zonghan Xie,Jian Ku Shang,Eric Formo,Pedro H. C. Camargo,Feng Fang,Jianqing Jiang
出处
期刊:Advanced Materials [Wiley]
卷期号:35 (45) 被引量:46
标识
DOI:10.1002/adma.202304494
摘要

Prussian blue analogs (PBAs) are promising catalysts for green hydrogen production. However, the rational design of high-performing PBAs is challenging, which requires an in-depth understanding of the catalytic mechanism. Here FeMn@CoNi core-shell PBAs are employed as precursors, together with Se powders, in low-temperature pyrolysis in an argon atmosphere. This synthesis method enables the partial dissociation of inner FeMn PBAs that results in hollow interiors, Ni nanoparticles (NPs) exsolution to the surface, and Se incorporation onto the PBA shell. The resulting material presents ultralow oxygen evolution reaction (OER) overpotential (184 mV at 10 mA cm-2 ) and low Tafel slope (43.4 mV dec-1 ), outperforming leading-edge PBA-based electrocatalysts. The mechanism responsible for such a high OER activity is revealed, assisted by density functional theory (DFT) calculations and the surface examination before and after the OER process. The exsolved Ni NPs are found to help turn the PBAs into Se-doped core-shell metal oxyhydroxides during the OER, in which the heterojunction with Ni and the Se incorporation are combined to improve the OER kinetics. This work shows that efficient OER catalysts could be developed by using a novel synthesis method backed up by a sound understanding and control of the catalytic pathway.
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