Revealing of Active Sites and Catalytic Mechanism in N-Coordinated Fe, Ni Dual-Doped Carbon with Superior Acidic Oxygen Reduction than Single-Atom Catalyst

Yaodan Zhou, Wen Yang*, Wellars Utetiwabo, Yi Meng Lian, Xue Yin, Lei Zhou, Peiwen Yu, Renjie Chen, Shaorui Sun

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

150 引用 (Scopus)

摘要

Herein, we synthesized a Fe, Ni dual-metal embedded in porous nitrogen-doped carbon material to endow higher turnover frequency (TOF), lower H2O2 yield, and thus superior durability than for the single-Atom catalyst for oxygen reduction in acid media. Quantitative X-ray absorption near edge structure (XANES) fitting and density functional theory (DFT) calculation were implemented to explore the active sites in the catalysts. The results suggest FeNi-N6 with type I (each metal atom coordinated with four nitrogen atoms) instead of type II configuration (each metal atom coordinated with three nitrogen atoms) dominates the catalytic activity of the noble-metal free catalyst (NMFC). Further, theoretical calculation reveals that the oxygen reduction reaction (ORR) activity trend of different moieties was FeNi-N6 (type I) > FeNi-N6 (type II) > Fe-N4 > Fe2-N6. Our research represents an important step for developing dual-metal doping NMFC for proton exchange membrane fuel cells (PEMFCs) by revealing its new structural configuration and correlation with catalytic activity.

源语言英语
页(从-至)1404-1410
页数7
期刊Journal of Physical Chemistry Letters
11
4
DOI
出版状态已出版 - 20 2月 2020

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Zhou, Y., Yang, W., Utetiwabo, W., Lian, Y. M., Yin, X., Zhou, L., Yu, P., Chen, R., & Sun, S. (2020). Revealing of Active Sites and Catalytic Mechanism in N-Coordinated Fe, Ni Dual-Doped Carbon with Superior Acidic Oxygen Reduction than Single-Atom Catalyst. Journal of Physical Chemistry Letters, 11(4), 1404-1410. https://doi.org/10.1021/acs.jpclett.9b03771