jp710498v_si_001.pdf (73.92 kB)
Noncovalent Assembly of a Metalloporphyrin and an Iron Hydrogenase Active-Site Model: Photo-Induced Electron Transfer and Hydrogen Generation
journal contributionposted on 2008-07-10, 00:00 authored by Xueqiang Li, Mei Wang, Suping Zhang, Jingxi Pan, Yong Na, Jianhui Liu, Björn Åkermark, Licheng Sun
A noncovalent assembly of a pyridyl-functionalized hydrogenase active-site model complex and zinc tetraphenylporphyrin has been obtained and characterized. Upon light irradiation, fluorescence quenching by electron transfer was observed from the singlet excited state of the porphyrin to the diiron center, and the mechanism was verified by fluorescence lifetime and transient absorption spectroscopic measurements. In contrast to molecular dyads linked by covalent bonds, the assembled system was designed to avoid charge recombination via complex dissociation after photo-induced electron transfer. Visible light-driven hydrogen generation was observed from this self-assembled system. The assembling strategy employed in this study has the potential to be used for any other hydrogenase models in the future.
light irradiationgenerationfluorescence quenchinghydrogenase modelsHydrogen GenerationA noncovalent assemblyelectron transferNoncovalent Assemblydiiron centermechanismstrategyElectronTransfercovalent bondszinc tetraphenylporphyrinfluorescence lifetimesingletcharge recombinationabsorption spectroscopic measurementsModelVisibledyaddissociationHydrogenasefuturecontrastMetalloporphyrin