The combination of o-phenylenediamine (opda), which possesses two
proton- and electron-pooling capability, with Fe(II) leads to the photochemical hydrogenevolution
reaction (HER) in THF at room temperature without addition of
photosensitizers. From the THF solution, the tris(o-phenylenediamine) iron(II) complex,
[FeII(opda)3](ClO4)2 (1), was isolated as a photoactive species, while the deprotonated
oxidized species was characterized by X-ray crystallographic analysis, electrospray
ionization mass spectrometry, and UV−vis NIR spectra. Furthermore, the HER is photocatalyzed by hydroquinone, which
serves as a H+/e− donor. The present work demonstrates that the use of a metal-bound aromatic amine as a H+/e− pooler opens
an alternative strategy for designing nonprecious-metal-based molecular photochemical H2 production/storage materials.
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