期刊
ADVANCED ENERGY MATERIALS
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202300961
关键词
2D SBU; charge separation; hydrogen; mechanism; photocatalysis; Ti-MOF
COK-47 is a promising metal-organic framework (MOF) for photocatalytic water splitting. It exhibits high activity and is responsive to visible light. The study demonstrates that particle morphology, surface area, and missing ligand defects are crucial parameters affecting the material's performance. COK-47(ISO) is among the most active MOFs to date, achieving a hydrogen evolution rate of 8.6 μmol h(-1) and an apparent quantum yield of 0.5% under visible light illumination.
Metal-organic frameworks (MOFs) are promising materials for photocatalytic water splitting reactions, but examples of visible light-responsive, catalytically active, and stable MOFs are still rare. A detailed investigation is conducted for COK-47 - a recently described MOF comprising 2D Ti-O-6 secondary building units (SBUs) - toward a photocatalytic hydrogen evolution reaction (HER), showing how overall particle morphology, surface area, and missing ligand defects are central parameters governing the material's ultimate performance. The newly synthesized COK-47(ISO) is among the most active MOFs to date, yielding HER-rates of 8.6 & mu;mol h(-1), and an apparent quantum yield (AQY) of 0.5% under visible light illumination. Optoelectronic and photoluminescence investigations, supported by theoretical calculations, enable the unraveling of its electronic structure along with charge transfer and recombination kinetics. A wavelength-dependent reaction mechanism is proposed involving ligand to metal charge transfer (LMCT) and the main challenges for visible or UV photoexcitation are identified, demonstrating that the unique 2D layered structure aids charge separation and is key to the high performance. This work introduces COK-47 as a promising alternative to the well-known MIL-125 family and offers directions for future studies
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