CAS OpenIR  > 中科院上海应用物理研究所2011-2019年
Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis
Shen, HJ; Gracia-Espino, E; Ma, JY; Tang, HD; Mamat, X; Wagberg, T; Hu, GZ; Guo, SJ
2017
Source PublicationNANO ENERGY
ISSN2211-2855
Volume35Pages:9-16
Subtype期刊论文
AbstractEarth-abundant materials with Fe-N-C centers have been identified as promising catalysts for oxygen reduction reaction (ORR), but these alternatives for Pt catalysts are usually the porphyrin-like FeN4 configuration. The density functional theory (DFT) calculations reveal that FeN2 outperforms FeN4 due to its lower interaction with *O-2 and *OH intermediates and enhanced electron transport, however, achieving an optimum design of these earth-abundant materials with the enriched FeN2 catalytic centers is still a great challenge. Here, we report an intriguing template casting strategy to introduce a mass of atomically dispersed FeN2 moieties onto the surface of N-doped ordered mesoporous carbon for boosting ORR electrocatalysis. One of unique parts herein is to pre anchor Fe precursor on the surface of template (SBA-15) during catalyst synthesis, preventing Fe from penetrating into the carbon skeleton and facilitating the removal of excessive Fe-based particles during silica elimination by HF etching, resulting in a desirable model structure comprising only highly active atomically dispersed FeN2 sites, as confirmed by high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), extended X-ray absorption fine structure (EXAFS) and Mossbauer spectroscopy analysis. The well-defined structure prompts us to understand the nature of the catalytic active sites, and to demonstrate that the catalyst activity is linearly proportional to the concentration of FeN2 sites. The obtained atomic electrocatalyst exhibits superior electrocatalytic performance for ORR with a more positive half-wave potential than that of Pt/C catalyst. We further establish a kinetic model to predict the ORR activity of these single-atom dispersed catalysts. The present work elaborates on a profound understanding for designing low-cost, highly efficient FeN2-based electrocatalyst for boosting ORR.
KeywordFen2 Atomic Dispersion Oxygen Reduction Reaction Kinetic Model Nitrogen-doped Carbon
DOI10.1016/j.nanoen.2017.03.027
Indexed BySCI
Language英语
WOS IDWOS:000400647900002
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/27261
Collection中科院上海应用物理研究所2011-2019年
Recommended Citation
GB/T 7714
Shen, HJ,Gracia-Espino, E,Ma, JY,et al. Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis[J]. NANO ENERGY,2017,35:9-16.
APA Shen, HJ.,Gracia-Espino, E.,Ma, JY.,Tang, HD.,Mamat, X.,...&Guo, SJ.(2017).Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis.NANO ENERGY,35,9-16.
MLA Shen, HJ,et al."Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis".NANO ENERGY 35(2017):9-16.
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