Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation
Abstract Coordination complexes are promising candidates for powerful electrocatalytic oxygen evolution reaction but challenges remain in favoring the kinetics behaviors through local coordination regulation. Herein, by refining the synergy of carboxylate anions and multiconjugated benzimidazole lig...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-12-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55120-1 |
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| author | Geng Zhang Wei Guo Hong Zheng Xiang Li Jinxin Wang Qiuyu Zhang |
| author_facet | Geng Zhang Wei Guo Hong Zheng Xiang Li Jinxin Wang Qiuyu Zhang |
| author_sort | Geng Zhang |
| collection | DOAJ |
| description | Abstract Coordination complexes are promising candidates for powerful electrocatalytic oxygen evolution reaction but challenges remain in favoring the kinetics behaviors through local coordination regulation. Herein, by refining the synergy of carboxylate anions and multiconjugated benzimidazole ligands, we tailor a series of well-defined and stable coordination complexes with three-dimensional supramolecular/coordinated structures. The coordinated water as potential open coordination sites can directly become intermediates, while the metal center easily achieves re-coordination with water molecules in the pores to resist lattice oxygen dissolution. In situ experiments and theory simulations indicate that nickel centers with neighboring coordinated water molecules follow an intramolecular oxygen coupling mechanism with a low thermodynamic energy barrier. With more coordinated water introduced, an optimized intramolecular oxygen coupling process may appear for favoring the reaction kinetics. As such, a low overpotential of 248 mV at 10 mA cm–2 and long-term stability of 200 h are achieved. This study underscores the potential of crafting coordinated water molecules for efficient electrocatalysis applications. |
| format | Article |
| id | doaj-art-8b9d6478b6ee46d7a16cc52c657e28a6 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-8b9d6478b6ee46d7a16cc52c657e28a62025-01-05T12:35:07ZengNature PortfolioNature Communications2041-17232024-12-0115111110.1038/s41467-024-55120-1Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidationGeng Zhang0Wei Guo1Hong Zheng2Xiang Li3Jinxin Wang4Qiuyu Zhang5Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityAbstract Coordination complexes are promising candidates for powerful electrocatalytic oxygen evolution reaction but challenges remain in favoring the kinetics behaviors through local coordination regulation. Herein, by refining the synergy of carboxylate anions and multiconjugated benzimidazole ligands, we tailor a series of well-defined and stable coordination complexes with three-dimensional supramolecular/coordinated structures. The coordinated water as potential open coordination sites can directly become intermediates, while the metal center easily achieves re-coordination with water molecules in the pores to resist lattice oxygen dissolution. In situ experiments and theory simulations indicate that nickel centers with neighboring coordinated water molecules follow an intramolecular oxygen coupling mechanism with a low thermodynamic energy barrier. With more coordinated water introduced, an optimized intramolecular oxygen coupling process may appear for favoring the reaction kinetics. As such, a low overpotential of 248 mV at 10 mA cm–2 and long-term stability of 200 h are achieved. This study underscores the potential of crafting coordinated water molecules for efficient electrocatalysis applications.https://doi.org/10.1038/s41467-024-55120-1 |
| spellingShingle | Geng Zhang Wei Guo Hong Zheng Xiang Li Jinxin Wang Qiuyu Zhang Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation Nature Communications |
| title | Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| title_full | Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| title_fullStr | Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| title_full_unstemmed | Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| title_short | Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| title_sort | identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation |
| url | https://doi.org/10.1038/s41467-024-55120-1 |
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