Promoted self-construction of beta-NiOOH in amorphous high entropy electrocatalysts for the oxygen evolution reaction

Han, Mei ¹Wang, Changhong ²Zhong, Jun ³Han, Jingrui ¹Wang, Ning ¹Seifitokaldani, Ali ⁴Yu, Yifu ²Liu, Yongchang ¹Sun, Xuhui ³Vomiero, Alberto ⁵Liang, Hongyan¹

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作者信息

1. Tianjin Univ, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China
2. Tianjin Univ, Inst Mol Plus, Tianjin 300072, Peoples R China
3. Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Suzhou 215123, Peoples R China
4. McGill Univ, Dept Chem Engn, Montreal, PQ H3A 0C5, Canada
5. Lulea Univ Technol, Dept Engn Sci & Math, Div Mat Sci, S-97187 Lulea, Sweden
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Abstract

The exploration of an efficient electrocatalyst for the oxygen evolution reaction (OER) is urgently required for sustainable renewable-energy conversion and storage. Due to the increased chemical complexity, multimetallic catalysts provide flexibility to alter their electronic and crystal structure to attain a superior intrinsic catalytic activity via synergistic effects, which is seldom accomplished using single metal catalysts. However, the high chemical complexity increases the difficulty to prepare elemental homogenous catalysts and reveal their synergistic effect during OER process, which further hinder the design of multimetallic catalysts. Here, high entropy concept is utilized to design an NiFeCoMnAl oxide with amorphous structure as OER catalyst. The direct evidence of active Ni sites is provided by the operando Raman measurements and Fe can modify oxygen intermediates binding energy on Ni sites. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) reveal that the incorporation of Mn can construct the electron-rich environment of active Ni center, and the relatively lower oxidation state of Ni facilitates the self-construction of beta-NiOOH intermediates, which shows promoted OER activity as confirmed by density functional theory calculations. Doping Co can enhance the conductivity and doping Al leads to the formation of nanoporous structure through dealloying process, thus each component is essential for improving OER performance. The optimized NiFeCoMnAl catalyst exhibits an overpotential of 190 mV at 10 mA cm(-2) in 1 M KOH solution, much superior to the ternary and quaternary counterparts. This work sheds light on understanding the origin of high entropy catalysts' OER activity and thereby enables the rational design of multinary transition metallic catalysts.

Key words

High entropy catalysts/Oxygen evolution reaction/Self-construction of beta-NiOOH intermediates/Amorphous nanoporous structure

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出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量95

参考文献量55

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