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

doi:10.1021/acs.jpclett.9b03771

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

J Phys Chem Lett. 2020 Feb 20;11(4):1404-1410. doi: 10.1021/acs.jpclett.9b03771. Epub 2020 Feb 6.

Authors

Yaodan Zhou¹, Wen Yang¹, Wellars Utetiwabo¹, Yi-Meng Lian¹, Xue Yin¹, Lei Zhou¹, Peiwen Yu¹, Renjie Chen², Shaorui Sun³

Affiliations

¹ Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering , Beijing Institute of Technology , Beijing 100081 , P. R. China.
² School of Material Science and Engineering , Beijing Institute of Technology , Beijing 100081 , P. R. China.
³ Beijing Key Laboratory for Green Catalysis and Separation, College of Environmental and Energy Engineering , Beijing University of Technology , Beijing 100124 , P. R. China.

PMID: 32004006
DOI: 10.1021/acs.jpclett.9b03771

Abstract

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.