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Fluorination of Covalent Organic Framework Reinforcing the Confinement of Pd Nanoclusters Enhances Hydrogen Peroxide Photosynthesis.
- Source :
-
Journal of the American Chemical Society [J Am Chem Soc] 2023 Sep 13; Vol. 145 (36), pp. 19877-19884. Date of Electronic Publication: 2023 Aug 16. - Publication Year :
- 2023
-
Abstract
- Metal-isolated clusters (MICs) physically confined on photoactive materials are of great interest in the field of photosynthesis of hydrogen peroxide (H <subscript>2</subscript> O <subscript>2</subscript> ). Despite recent important endeavors, weak confinement of MICs in the reported photocatalytic systems leads to their low catalytic activity and stability. Herein, we report a new strategy of fluorinated covalent organic frameworks (COFs) to strongly confine Pd ICs for greatly boosting the photocatalytic activity and stability of H <subscript>2</subscript> O <subscript>2</subscript> photosynthesis. Both experimental and theoretical results reveal that strong electronegative fluorine can increase the metal-support interaction and optimize the d-band center of Pd ICs, thus significantly enhancing the stability and activity of photocatalytic H <subscript>2</subscript> O <subscript>2</subscript> . An optimal TAPT-TFPA COFs@Pd ICs photocatalyst delivers a stable H <subscript>2</subscript> O <subscript>2</subscript> yield rate of 2143 μmol h <superscript>-1</superscript> g <superscript>-1</superscript> . Most importantly, the as-made TAPT-TFPA COFs@Pd ICs exhibit high catalytic stability over 100 h, which is the best among the reported materials.
Details
- Language :
- English
- ISSN :
- 1520-5126
- Volume :
- 145
- Issue :
- 36
- Database :
- MEDLINE
- Journal :
- Journal of the American Chemical Society
- Publication Type :
- Academic Journal
- Accession number :
- 37584527
- Full Text :
- https://doi.org/10.1021/jacs.3c05914