High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands
Abstract Recent studies have shown that single- or few-atom catalysts, with local states near the Fermi level, can promote nitrogen activation and the entire electrocatalytic nitrogen reduction reaction (eNRR) process, but are facing limitations in loading densities and stability. Here, we conceptua...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-05-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-025-01663-w |
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| author | Yuyuan Huang Yanru Chen Shunhong Zhang Zhenyu Zhang Ping Cui |
| author_facet | Yuyuan Huang Yanru Chen Shunhong Zhang Zhenyu Zhang Ping Cui |
| author_sort | Yuyuan Huang |
| collection | DOAJ |
| description | Abstract Recent studies have shown that single- or few-atom catalysts, with local states near the Fermi level, can promote nitrogen activation and the entire electrocatalytic nitrogen reduction reaction (eNRR) process, but are facing limitations in loading densities and stability. Here, we conceptualize that the Kagome metals featuring naturally abundant surface sites and flat bands are promising candidates to catalyze eNRR. Using first-principles calculations, we first show that the Kagome termination of the prototypical FeSn is accompanied by the presence of flat bands from the Fe-d z² and d xz/d yz orbitals, and the exposed surface can strongly chemisorb N2 with an adsorption energy of ~−0.7 eV. The limiting potential of 0.31 V indicates superior eNRR catalytic activity. The mutual independence between neighboring reactive sites also ensures an exceptionally high 25% atomic utilization within the Kagome layer, with each active site possessing high selectivity of eNRR. Our detailed analysis further reveals the critical role of the flat bands in boosting catalytic activity, which is also generalized to the isostructural CoSn and FeGe Kagome systems. Collectively, this work not only enhances the functionalities of Kagome materials for applications but also integrates flat band physics with single-atom catalysis, offering new opportunities in catalyst design. |
| format | Article |
| id | doaj-art-d509fa2f8cb349d8a36e8e4667282f4c |
| institution | OA Journals |
| issn | 2057-3960 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
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| series | npj Computational Materials |
| spelling | doaj-art-d509fa2f8cb349d8a36e8e4667282f4c2025-08-20T02:03:36ZengNature Portfolionpj Computational Materials2057-39602025-05-011111810.1038/s41524-025-01663-wHigh-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bandsYuyuan Huang0Yanru Chen1Shunhong Zhang2Zhenyu Zhang3Ping Cui4International Center for Quantum Design of Functional Materials (ICQD), Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaInternational Center for Quantum Design of Functional Materials (ICQD), Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaInternational Center for Quantum Design of Functional Materials (ICQD), Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaInternational Center for Quantum Design of Functional Materials (ICQD), Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaInternational Center for Quantum Design of Functional Materials (ICQD), Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaAbstract Recent studies have shown that single- or few-atom catalysts, with local states near the Fermi level, can promote nitrogen activation and the entire electrocatalytic nitrogen reduction reaction (eNRR) process, but are facing limitations in loading densities and stability. Here, we conceptualize that the Kagome metals featuring naturally abundant surface sites and flat bands are promising candidates to catalyze eNRR. Using first-principles calculations, we first show that the Kagome termination of the prototypical FeSn is accompanied by the presence of flat bands from the Fe-d z² and d xz/d yz orbitals, and the exposed surface can strongly chemisorb N2 with an adsorption energy of ~−0.7 eV. The limiting potential of 0.31 V indicates superior eNRR catalytic activity. The mutual independence between neighboring reactive sites also ensures an exceptionally high 25% atomic utilization within the Kagome layer, with each active site possessing high selectivity of eNRR. Our detailed analysis further reveals the critical role of the flat bands in boosting catalytic activity, which is also generalized to the isostructural CoSn and FeGe Kagome systems. Collectively, this work not only enhances the functionalities of Kagome materials for applications but also integrates flat band physics with single-atom catalysis, offering new opportunities in catalyst design.https://doi.org/10.1038/s41524-025-01663-w |
| spellingShingle | Yuyuan Huang Yanru Chen Shunhong Zhang Zhenyu Zhang Ping Cui High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands npj Computational Materials |
| title | High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands |
| title_full | High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands |
| title_fullStr | High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands |
| title_full_unstemmed | High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands |
| title_short | High-density natural active sites for efficient nitrogen reduction on Kagome surfaces promoted by flat bands |
| title_sort | high density natural active sites for efficient nitrogen reduction on kagome surfaces promoted by flat bands |
| url | https://doi.org/10.1038/s41524-025-01663-w |
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