A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting
Abstract Here, a sol‐gel method is used to prepare a Prussian blue analogue (NiFe‐PBA) precursor with a 2D network, which is further annealed to an Fe3O4/NiCx composite (NiFe‐PBA‐gel‐cal), inheriting the ultrahigh specific surface area of the parent structure. When the composite is used as both anod...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2022-05-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202200146 |
| _version_ | 1817986757344362496 |
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| author | Hao Zhang Songyuan Geng Mengzheng Ouyang Hossein Yadegari Fang Xie D. Jason Riley |
| author_facet | Hao Zhang Songyuan Geng Mengzheng Ouyang Hossein Yadegari Fang Xie D. Jason Riley |
| author_sort | Hao Zhang |
| collection | DOAJ |
| description | Abstract Here, a sol‐gel method is used to prepare a Prussian blue analogue (NiFe‐PBA) precursor with a 2D network, which is further annealed to an Fe3O4/NiCx composite (NiFe‐PBA‐gel‐cal), inheriting the ultrahigh specific surface area of the parent structure. When the composite is used as both anode and cathode catalyst for overall water splitting, it requires low voltages of 1.57 and 1.66 V to provide a current density of 100 mA cm−2 in alkaline freshwater and simulated seawater, respectively, exhibiting no obvious attenuation over a 50 h test. Operando Raman spectroscopy and X‐ray photoelectron spectroscopy indicate that NiOOH2–x active species containing high‐valence Ni3+/Ni4+ are in situ generated from NiCx during the water oxidation. Density functional theory calculations combined with ligand field theory reveal that the role of high valence states of Ni is to trigger the production of localized O 2p electron holes, acting as electrophilic centers for the activation of redox reactions for oxygen evolution reaction. After hydrogen evolution reaction, a series of ex situ and in situ investigations indicate the reduction from Fe3+ to Fe2+ and the evolution of Ni(OH)2 are the origin of the high activity. |
| first_indexed | 2024-04-14T00:13:33Z |
| format | Article |
| id | doaj.art-a976194308914fbb8557a0a944dabf1b |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-04-14T00:13:33Z |
| publishDate | 2022-05-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-a976194308914fbb8557a0a944dabf1b2022-12-22T02:23:13ZengWileyAdvanced Science2198-38442022-05-01915n/an/a10.1002/advs.202200146A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater SplittingHao Zhang0Songyuan Geng1Mengzheng Ouyang2Hossein Yadegari3Fang Xie4D. Jason Riley5Department of Materials and London Center for Nanotechnology Imperial College London London SW7 2AZ UKDepartment of Chemistry Imperial College London London SW7 2AZ UKDepartment of Earth Science and Engineering Imperial College London London SW7 2AZ UKDepartment of Materials and London Center for Nanotechnology Imperial College London London SW7 2AZ UKDepartment of Materials and London Center for Nanotechnology Imperial College London London SW7 2AZ UKDepartment of Materials and London Center for Nanotechnology Imperial College London London SW7 2AZ UKAbstract Here, a sol‐gel method is used to prepare a Prussian blue analogue (NiFe‐PBA) precursor with a 2D network, which is further annealed to an Fe3O4/NiCx composite (NiFe‐PBA‐gel‐cal), inheriting the ultrahigh specific surface area of the parent structure. When the composite is used as both anode and cathode catalyst for overall water splitting, it requires low voltages of 1.57 and 1.66 V to provide a current density of 100 mA cm−2 in alkaline freshwater and simulated seawater, respectively, exhibiting no obvious attenuation over a 50 h test. Operando Raman spectroscopy and X‐ray photoelectron spectroscopy indicate that NiOOH2–x active species containing high‐valence Ni3+/Ni4+ are in situ generated from NiCx during the water oxidation. Density functional theory calculations combined with ligand field theory reveal that the role of high valence states of Ni is to trigger the production of localized O 2p electron holes, acting as electrophilic centers for the activation of redox reactions for oxygen evolution reaction. After hydrogen evolution reaction, a series of ex situ and in situ investigations indicate the reduction from Fe3+ to Fe2+ and the evolution of Ni(OH)2 are the origin of the high activity.https://doi.org/10.1002/advs.202200146iron oxidelattice oxygennickel carbideseawater splittingself‐reconstruction |
| spellingShingle | Hao Zhang Songyuan Geng Mengzheng Ouyang Hossein Yadegari Fang Xie D. Jason Riley A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting Advanced Science iron oxide lattice oxygen nickel carbide seawater splitting self‐reconstruction |
| title | A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting |
| title_full | A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting |
| title_fullStr | A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting |
| title_full_unstemmed | A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting |
| title_short | A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide @ Iron Oxide Network for Seawater Splitting |
| title_sort | self reconstructed bifunctional electrocatalyst of pseudo amorphous nickel carbide iron oxide network for seawater splitting |
| topic | iron oxide lattice oxygen nickel carbide seawater splitting self‐reconstruction |
| url | https://doi.org/10.1002/advs.202200146 |
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