Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts
Single-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support for the rational design of single-si...
| المؤلفون الرئيسيون: | , , , , , , , , |
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| التنسيق: | Journal article |
| اللغة: | English |
| منشور في: |
Springer Nature
2021
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| _version_ | 1826258150101090304 |
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| author | Wan, W Zhao, Y Wei, S Triana, CA Li, J Arcifa, A Allen, CS Cao, R Patzke, GR |
| author_facet | Wan, W Zhao, Y Wei, S Triana, CA Li, J Arcifa, A Allen, CS Cao, R Patzke, GR |
| author_sort | Wan, W |
| collection | OXFORD |
| description | Single-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support for the rational design of single-site and dual-site single-atom catalysts. Catalysts with single Fe sites exhibit impressive oxygen reduction reaction activity with a half-wave potential of 0.89 V vs. RHE. We find that the single Ni sites are favorable to promote the key structural reconstruction into bridging Ni-O-Fe bonds in dual-site NiFe SAC. Meanwhile, the newly formed Ni-O-Fe bonds create spin channels for electron transfer, resulting in a significant improvement of the oxygen evolution reaction activity with an overpotential of 270 mV at 10 mA cm−2. We further reveal that the water oxidation reaction follows a dual-site pathway through the deprotonation of *OH at both Ni and Fe sites, leading to the formation of bridging O2 atop the Ni-O-Fe sites.
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| first_indexed | 2024-03-06T18:29:28Z |
| format | Journal article |
| id | oxford-uuid:0925997a-d6ac-464f-a81b-b3d7b1cf53c4 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T18:29:28Z |
| publishDate | 2021 |
| publisher | Springer Nature |
| record_format | dspace |
| spelling | oxford-uuid:0925997a-d6ac-464f-a81b-b3d7b1cf53c42022-03-26T09:16:40ZMechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalystsJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:0925997a-d6ac-464f-a81b-b3d7b1cf53c4EnglishSymplectic ElementsSpringer Nature2021Wan, WZhao, YWei, STriana, CALi, JArcifa, AAllen, CSCao, RPatzke, GRSingle-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support for the rational design of single-site and dual-site single-atom catalysts. Catalysts with single Fe sites exhibit impressive oxygen reduction reaction activity with a half-wave potential of 0.89 V vs. RHE. We find that the single Ni sites are favorable to promote the key structural reconstruction into bridging Ni-O-Fe bonds in dual-site NiFe SAC. Meanwhile, the newly formed Ni-O-Fe bonds create spin channels for electron transfer, resulting in a significant improvement of the oxygen evolution reaction activity with an overpotential of 270 mV at 10 mA cm−2. We further reveal that the water oxidation reaction follows a dual-site pathway through the deprotonation of *OH at both Ni and Fe sites, leading to the formation of bridging O2 atop the Ni-O-Fe sites. |
| spellingShingle | Wan, W Zhao, Y Wei, S Triana, CA Li, J Arcifa, A Allen, CS Cao, R Patzke, GR Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title | Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title_full | Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title_fullStr | Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title_full_unstemmed | Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title_short | Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts |
| title_sort | mechanistic insight into the active centers of single dual atom ni fe based oxygen electrocatalysts |
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