Details

Autor(en) / Beteiligte

• Shen, Hangjia
• Gracia-Espino, Eduardo
• Ma, Jingyuan
• Tang, Haodong
• Mamat, Xamxikamar
• Wagberg, Thomas
• Hu, Guangzhi
• Guo, Shaojun

Titel

Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis

Ist Teil von

• Nano energy, 2017-05, Vol.35, p.9-16

Ort / Verlag

Elsevier Ltd

Erscheinungsjahr

2017

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• 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 *O2 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 Mößbauer 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. A new class of atomically FeN2 moieties dispersed on the surface of N-doped mesoporous carbon were prepared via template casting procedure as highly efficient electrocatalysts for boosting oxygen reduction. The regulation of mononuclear FeN2 moieties (an active site toward four-electron process) can linearly increase the ORR activity. [Display omitted] •A template casting method to introduce ORR catalytic sites FeN2 atomically dispersed on the surface of ordered mesoporous carbon support.•A higher ORR activity with enhanced stability is achieved, and a kinetic model is established to predict the ORR activity.•Density functional theory calculations reveal higher ORR activity and enhanced electron transport of FeN2 than FeN4 moieties.