The role of iron nitrides in the Fe–N–C catalysis system towards the oxygen reduction reaction
Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N moieties, leading to controversial contributio...
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| Published in | Nanoscale Vol. 9; no. 22; pp. 7641 - 7649 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
2017
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N
moieties, leading to controversial contributions of these components to the catalysis of the ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, Fe
N nanoparticles (NPs) embedded in mesoporous N-doped carbon without Fe-N
moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterization (especially from Mössbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on the main surfaces of Fe
N including ε-Fe
N and ζ-Fe
N, it can be deduced that Fe
N NPs as active species make a contribution to the ORR catalysis, of which ε-Fe
N (x ≤ 2.1) is more active than ζ-Fe
N. In addition, we find that there exists an obvious synergistic effect between Fe
N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity. |
|---|---|
| AbstractList | Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N
moieties, leading to controversial contributions of these components to the catalysis of the ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, Fe
N nanoparticles (NPs) embedded in mesoporous N-doped carbon without Fe-N
moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterization (especially from Mössbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on the main surfaces of Fe
N including ε-Fe
N and ζ-Fe
N, it can be deduced that Fe
N NPs as active species make a contribution to the ORR catalysis, of which ε-Fe
N (x ≤ 2.1) is more active than ζ-Fe
N. In addition, we find that there exists an obvious synergistic effect between Fe
N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity. Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N4 moieties, leading to controversial contributions of these components to the catalysis of the ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, FexN nanoparticles (NPs) embedded in mesoporous N-doped carbon without Fe-N4 moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterization (especially from Mössbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on the main surfaces of Fe2N including ε-Fe2N and ζ-Fe2N, it can be deduced that Fe2N NPs as active species make a contribution to the ORR catalysis, of which ε-FexN (x ≤ 2.1) is more active than ζ-Fe2N. In addition, we find that there exists an obvious synergistic effect between Fe2N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity.Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N4 moieties, leading to controversial contributions of these components to the catalysis of the ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, FexN nanoparticles (NPs) embedded in mesoporous N-doped carbon without Fe-N4 moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterization (especially from Mössbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on the main surfaces of Fe2N including ε-Fe2N and ζ-Fe2N, it can be deduced that Fe2N NPs as active species make a contribution to the ORR catalysis, of which ε-FexN (x ≤ 2.1) is more active than ζ-Fe2N. In addition, we find that there exists an obvious synergistic effect between Fe2N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity. Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of various components such as iron nitrides, metallic iron, iron carbides, N-doped carbon and Fe-N4 moieties, leading to controversial contributions of these components to the catalysis of the ORR, especially iron nitrides. In this work, to investigate the function of iron nitrides, FexN nanoparticles (NPs) embedded in mesoporous N-doped carbon without Fe-N4 moieties are designed and constructed by a simple histidine-assisted method. Herein, the use of histidine can increase the N and Fe contents in the product. The obtained catalyst exhibits excellent ORR catalytic activity which is very close to that of the commercial Pt/C catalyst in alkaline electrolytes. Combining the catalytic activity, structural characterization (especially from Mossbauer spectroscopy), and the results of DFT calculations for adsorption energies of oxygen on the main surfaces of Fe2N including epsilon -Fe2N and zeta -Fe2N, it can be deduced that Fe2N NPs as active species make a contribution to the ORR catalysis, of which epsilon -FexN (x less than or equal to 2.1) is more active than zeta -Fe2N. In addition, we find that there exists an obvious synergistic effect between Fe2N NPs and N-doped carbon, leading to the greatly enhanced ORR catalytic activity. |
| Author | Mu, Shichun Yang, Yushi Pu, Zonghua Zhu, Peipei Wang, Min Kou, Zongkui Liu, Xiaobo |
| Author_xml | – sequence: 1 givenname: Min surname: Wang fullname: Wang, Min – sequence: 2 givenname: Yushi surname: Yang fullname: Yang, Yushi – sequence: 3 givenname: Xiaobo surname: Liu fullname: Liu, Xiaobo – sequence: 4 givenname: Zonghua surname: Pu fullname: Pu, Zonghua – sequence: 5 givenname: Zongkui orcidid: 0000-0002-5377-2376 surname: Kou fullname: Kou, Zongkui – sequence: 6 givenname: Peipei surname: Zhu fullname: Zhu, Peipei – sequence: 7 givenname: Shichun orcidid: 0000-0003-3902-0976 surname: Mu fullname: Mu, Shichun |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/28540947$$D View this record in MEDLINE/PubMed |
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| Snippet | Fe-N-C series catalysts are always attractive for their high catalytic activity towards the oxygen reduction reaction (ORR). However, they usually consist of... |
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| SubjectTerms | Carbon Catalysis Catalysts Catalytic activity Iron Iron nitride Nanoparticles Oxygen |
| Title | The role of iron nitrides in the Fe–N–C catalysis system towards the oxygen reduction reaction |
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