Journal
MICROPOROUS AND MESOPOROUS MATERIALS
Volume 355, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.micromeso.2023.112565
Keywords
Metal-organic framework; Surface diels-alder adducts; Ruthenium photosensitizer; Photocatalysis; Hydrogen evolution reaction
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A new heterogeneous photosensitizer, Ru@dpdhpzBASF-A520, was successfully synthesized through a unique strategy incorporating dipyridyl-dihydropyridazine adducts onto the aluminum fumarate units of highly porous MOF BASF-A520 and coordinating them to ruthenium metal centers. The resulting material displayed strong visible light absorption, allowing it to function as a single-site solid photosensitizer for hydrogen evolution in a photochemical reaction. Through various characterization techniques, it was confirmed that the ruthenium dipyridyl-dihydropyridazine adducts were effectively stabilized on the MOF surface and could efficiently inject electrons to Pt nanoparticles mediated by MV electron carrier for hydrogen generation from water.
A heterogeneous photosensitizer Ru@dpdhpzBASF-A520 has been successfully synthesized following an unprecedented strategy based on the incorporation of surface dipyridyl-dihydropyridazine adducts by Diels-Alder reaction on the aluminum fumarate units of the highly porous metal-organic framework (MOF) BASF-A520 and their further coordination to ruthenium metal centers. The characterization of the resulting metal-organic framework, including the ruthenium bipyridine-like photosensitizer moieties attached to its linkers, has been carried out by a wide variety of techniques, such as X-ray diffraction (XRD), transmission electron microscopy (TEM), nitrogen adsorption-desorption isotherms, solid-state cross-polarization magic angle spinning carbon-13 nuclear magnetic resonance (13C CP/MAS NMR), X-ray photoelectron spectroscopy (XPS) and ultraviolet-visible (UV-vis) spectroscopy. The light absorption in the visible region shown by the resulting material, Ru@dpdhpzBASF-A520, has allowed its application as a single-site solid photosensitizer for photochemical reactions of hydrogen evolution in conjunction with Pt nanoparticles as catalyst, EDTA as sacrificial electron donor and MV as electron carrier. A remarkable photocatalytic activity after 72 h was achieved, with a TON of 1157 based on the heterogeneous ruthenium photosensitizer, in aqueous solution at pH 5.0, which confirmed the effective stabilization of the ruthenium dipyridyl-dihydropyridazine adducts on the MOF surface and the efficient electron injection from the photoexcited Ru@dpdhpzBASF-A520 to Pt nanoparticles mediated by MV electron carrier for hydrogen generation from water.
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