| Title: | Non-covalent ligand-oxide interaction promotes oxygen evolution |
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| Authors: | ID Wu, Qianbao (Author)
ID Liang, Junwu (Author)
ID Xiao, Mengjun (Author)
ID Long, Chang (Author)
ID Li, Lei (Author)
ID Zeng, Zhenhua (Author)
ID Mavrič, Andraž (Author)
ID Zheng, Xia (Author)
ID Zhu, Jing (Author)
ID Valant, Matjaž (Author), et al. |
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| Files: |  RAZ_Wu_Qianbao_2023.pdf (1,77 MB)
MD5: E4F79C241FB1DD40A54149C271260491
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| Language: | English |
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| Work type: | Unknown |
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| Typology: | 1.01 - Original Scientific Article |
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| Organization: | UNG - University of Nova Gorica
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| Abstract: | Strategies to generate high-valence metal species capable of oxidizing water often employ composition and coordination tuning of oxide-based catalysts, where strong covalent interactions with metal sites are crucial. However, it remains unexplored whether a relatively weak “non-bonding” interaction between ligands and oxides can mediate the electronic states of metal sites in oxides. Here we present an unusual non-covalent phenanthroline-CoO2 interaction that substantially elevates the population of Co4+ sites for improved water oxidation. We find that phenanthroline only coordinates with Co2+ forming soluble Co(phenanthroline)2(OH)2 complex in alkaline electrolytes, which can be deposited as amorphous CoOxHy film containing non-bonding phenanthroline upon oxidation of Co2+ to Co3+/4+. This in situ deposited catalyst demonstrates a low overpotential of 216 mV at 10 mA cm−2 and sustainable activity over 1600 h with Faradaic efficiency above 97%. Density functional theory calculations reveal that the presence of phenanthroline can stabilize CoO2 through the non-covalent interaction and generate polaron-like electronic states at the Co-Co center. |
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| Keywords: | water oxidation, cobalt hydroxide, ligand-metal interactions |
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| Publication status: | Published |
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| Publication version: | Version of Record |
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| Publication date: | 01.01.2023 |
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| Year of publishing: | 2023 |
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| Number of pages: | str. 1-12 |
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| Numbering: | Vol. 14, article no. 997 |
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| PID: | 20.500.12556/RUNG-7997-ba085eca-51ea-1c45-6b79-1b60410f164f  |
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| COBISS.SI-ID: | 142729475 |
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| UDC: | 54 |
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| ISSN on article: | 2041-1723 |
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| DOI: | 10.1038/s41467-023-36718-3 |
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| NUK URN: | URN:SI:UNG:REP:TFCI9DZW |
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| Publication date in RUNG: | 23.02.2023 |
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| Views: | 3397 |
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| Downloads: | 19 |
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