Synergistic Effect of Bio-Inspired Microenvironment Modulation and Catalytic Site Design Enhances the Oxygen Evolution Performance of Copper-Phenanthroline Catalysts
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| Titel: | Synergistic Effect of Bio-Inspired Microenvironment Modulation and Catalytic Site Design Enhances the Oxygen Evolution Performance of Copper-Phenanthroline Catalysts |
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| Autoren: | Zhou, Mu-Han, Zheng, Tao, Li, Rui-Qi, Xie, Yi-Lin, Ruan, Gui-Lin, Dagnaw, Fentahun Wondu, Li, Xu-Bing, Wu, Zhixing, Tong, Qing-Xiao, Jian, Jing-Xin |
| Quelle: | CARBON ENERGY. |
| Schlagwörter: | carbon dots, copper complex, photovoltaic-electrolysis, solar conversion, water splitting |
| Beschreibung: | Copper complexes inspired by O2-activating enzymes have been widely investigated as molecular water oxidation catalysts, capable of facile and reversible O & horbar;O bond formation and cleavage under mild conditions. In this study, two copper phenanthroline complexes, namely, Cu(phen) and Cu(dophen), exhibit high turnover frequencies (TOFs) of 74 +/- 13 and (5.66 +/- 0.29) x 103 s-1 for water oxidation, respectively. Moreover, amino acid-functionalized carbon dots (CDs) were used to support the adhesion of the [Cu] complexes onto the electrode, significantly enhancing the TOFs of (2.80 +/- 0.12) x 103 and (4.11 +/- 0.24) x 104 s-1, respectively, exceeding the activity of photosystem II in nature. Remarkably, the amino acid-functionalized CDs provide a secondary sphere that mimics the catalytic microenvironment of the copper centre, which promotes proton-coupled electron transfer and O & horbar;O bond formation. Finally, the photovoltaic-electrolysis (PVE) system was established using CDs-supported Cu catalysts and commercial silicon solar panels, achieving a high solar-to-hydrogen efficiency of 11.59% under the illumination of AM 1.5 G. This represents the most efficient solar-driven water splitting system based on copper-based catalysts to date, introducing the biomimetic secondary sphere to a "proton-rocking" process for water oxidation catalysis and application of the PVE system. |
| Dateibeschreibung: | electronic |
| Zugangs-URL: | https://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-216493 https://doi.org/10.1002/cey2.70063 |
| Datenbank: | SwePub |
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Nájsť tento článok vo Web of Science | Abstract: | Copper complexes inspired by O2-activating enzymes have been widely investigated as molecular water oxidation catalysts, capable of facile and reversible O & horbar;O bond formation and cleavage under mild conditions. In this study, two copper phenanthroline complexes, namely, Cu(phen) and Cu(dophen), exhibit high turnover frequencies (TOFs) of 74 +/- 13 and (5.66 +/- 0.29) x 103 s-1 for water oxidation, respectively. Moreover, amino acid-functionalized carbon dots (CDs) were used to support the adhesion of the [Cu] complexes onto the electrode, significantly enhancing the TOFs of (2.80 +/- 0.12) x 103 and (4.11 +/- 0.24) x 104 s-1, respectively, exceeding the activity of photosystem II in nature. Remarkably, the amino acid-functionalized CDs provide a secondary sphere that mimics the catalytic microenvironment of the copper centre, which promotes proton-coupled electron transfer and O & horbar;O bond formation. Finally, the photovoltaic-electrolysis (PVE) system was established using CDs-supported Cu catalysts and commercial silicon solar panels, achieving a high solar-to-hydrogen efficiency of 11.59% under the illumination of AM 1.5 G. This represents the most efficient solar-driven water splitting system based on copper-based catalysts to date, introducing the biomimetic secondary sphere to a "proton-rocking" process for water oxidation catalysis and application of the PVE system. |
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| ISSN: | 26379368 |
| DOI: | 10.1002/cey2.70063 |