Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis
文献类型：期刊论文
| 作者 | Shen, HJ; Gracia-Espino, E; Ma, JY; Tang, HD; Mamat, X; Wagberg, T; Hu, GZ; Guo, SJ |
| 刊名 | NANO ENERGY
 |
| 出版日期 | 2017 |
| 卷号 | 35页码:9-16 |
| 关键词 | Fen2 Atomic Dispersion Oxygen Reduction Reaction Kinetic Model Nitrogen-doped Carbon |
| ISSN号 | 2211-2855 |
| DOI | 10.1016/j.nanoen.2017.03.027 |
| 文献子类 | 期刊论文 |
| 英文摘要 | Earth-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. |
| 语种 | 英语 |
| WOS记录号 | WOS:000400647900002 |
| 源URL | [http://ir.sinap.ac.cn/handle/331007/27261]  |
| 专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：上海应用物理研究所
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