FRINK Linked Data Fragments server

Matches in SemOpenAlex for { <https://semopenalex.org/work/W2009907754> ?p ?o ?g. }

• W2009907754 endingPage "5383" @default.
• W2009907754 startingPage "5373" @default.
• W2009907754 abstract "A pyridyl-functionalized diiron dithiolate complex, [μ-(4-pyCH2–NMI-S2)Fe2(CO)6] (3, py = pyridine (ligand), NMI = naphthalene monoimide) was synthesized and fully characterized. In the presence of zinc tetraphenylporphyrin (ZnTPP), a self-assembled 3·ZnTPP complex was readily formed in CH2Cl2 by the coordination of the pyridyl nitrogen to the porphyrin zinc center. Ultrafast photoinduced electron transfer from excited ZnTPP to complex 3 in the supramolecular assembly was observed in real time by monitoring the ν(C≡O) and ν(C═O)NMI spectral changes with femtosecond time-resolved infrared (TRIR) spectroscopy. We have confirmed that photoinduced charge separation produced the monoreduced species by comparing the time-resolved IR spectra with the conventional IR spectra of 3•– generated by reversible electrochemical reduction. The lifetimes for the charge separation and charge recombination processes were found to be τCS = 40 ± 3 ps and τCR = 205 ± 14 ps, respectively. The charge recombination is much slower than that in an analogous covalent complex, demonstrating the potential of a supramolecular approach to extend the lifetime of the charge-separated state in photocatalytic complexes. The observed vibrational frequency shifts provide a very sensitive probe of the delocalization of the electron-spin density over the different parts of the Fe2S2 complex. The TR and spectro-electrochemical IR spectra, electron paramagnetic resonance spectra, and density functional theory calculations all show that the spin density in 3•– is delocalized over the diiron core and the NMI bridge. This delocalization explains why the complex exhibits low catalytic dihydrogen production even though it features a very efficient photoinduced electron transfer. The ultrafast porphyrin-to-NMI-S2–Fe2(CO)6 photoinduced electron transfer is the first reported example of a supramolecular Fe2S2-hydrogenase model studied by femtosecond TRIR spectroscopy. Our results show that TRIR spectroscopy is a powerful tool to investigate photoinduced electron transfer in potential dihydrogen-producing catalytic complexes, and that way to optimize their performance by rational approaches." @default.
• W2009907754 created "2016-06-24" @default.
• W2009907754 creator A5013850715 @default.
• W2009907754 creator A5029252935 @default.
• W2009907754 creator A5033413143 @default.
• W2009907754 creator A5037093217 @default.
• W2009907754 creator A5042130936 @default.
• W2009907754 creator A5065419027 @default.
• W2009907754 creator A5069538040 @default.
• W2009907754 creator A5073070877 @default.
• W2009907754 date "2014-04-26" @default.
• W2009907754 modified "2023-10-16" @default.
• W2009907754 title "Direct Probing of Photoinduced Electron Transfer in a Self-Assembled Biomimetic [2Fe2S]-Hydrogenase Complex Using Ultrafast Vibrational Spectroscopy" @default.
• W2009907754 cites W1862448473 @default.
• W2009907754 cites W1971421347 @default.
• W2009907754 cites W1977101738 @default.
• W2009907754 cites W1979561954 @default.
• W2009907754 cites W1979791721 @default.
• W2009907754 cites W1982356449 @default.
• W2009907754 cites W1982792433 @default.
• W2009907754 cites W1985241764 @default.
• W2009907754 cites W1988091937 @default.
• W2009907754 cites W1990130563 @default.
• W2009907754 cites W1990633758 @default.
• W2009907754 cites W1994958725 @default.
• W2009907754 cites W2002891351 @default.
• W2009907754 cites W2005285870 @default.
• W2009907754 cites W2013082410 @default.
• W2009907754 cites W2023271753 @default.
• W2009907754 cites W2024225695 @default.
• W2009907754 cites W2024374247 @default.
• W2009907754 cites W2027591191 @default.
• W2009907754 cites W2030117598 @default.
• W2009907754 cites W2030687437 @default.
• W2009907754 cites W2035380505 @default.
• W2009907754 cites W2036154963 @default.
• W2009907754 cites W2036780929 @default.
• W2009907754 cites W2037229667 @default.
• W2009907754 cites W2042285340 @default.
• W2009907754 cites W2056872218 @default.
• W2009907754 cites W2060962014 @default.
• W2009907754 cites W2063074480 @default.
• W2009907754 cites W2065529333 @default.
• W2009907754 cites W2066255580 @default.
• W2009907754 cites W2068824954 @default.
• W2009907754 cites W2073160469 @default.
• W2009907754 cites W2073193293 @default.
• W2009907754 cites W2073508479 @default.
• W2009907754 cites W2075361563 @default.
• W2009907754 cites W2079436950 @default.
• W2009907754 cites W2083547736 @default.
• W2009907754 cites W2086249975 @default.
• W2009907754 cites W2086634861 @default.
• W2009907754 cites W2086957099 @default.
• W2009907754 cites W2089435321 @default.
• W2009907754 cites W2091258026 @default.
• W2009907754 cites W2102464022 @default.
• W2009907754 cites W2104796556 @default.
• W2009907754 cites W2109793613 @default.
• W2009907754 cites W2123068207 @default.
• W2009907754 cites W213791877 @default.
• W2009907754 cites W2138977251 @default.
• W2009907754 cites W2143981217 @default.
• W2009907754 cites W2150312271 @default.
• W2009907754 cites W2160989746 @default.
• W2009907754 cites W2162069512 @default.
• W2009907754 cites W2166162385 @default.
• W2009907754 cites W2171627829 @default.
• W2009907754 cites W2320062496 @default.
• W2009907754 cites W2323559321 @default.
• W2009907754 cites W2325173426 @default.
• W2009907754 cites W2327497300 @default.
• W2009907754 cites W3036723969 @default.
• W2009907754 cites W4247963155 @default.
• W2009907754 doi "https://doi.org/10.1021/ic500777d" @default.
• W2009907754 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/24766080" @default.
• W2009907754 hasPublicationYear "2014" @default.
• W2009907754 type Work @default.
• W2009907754 sameAs 2009907754 @default.
• W2009907754 citedByCount "41" @default.
• W2009907754 countsByYear W20099077542014 @default.
• W2009907754 countsByYear W20099077542015 @default.
• W2009907754 countsByYear W20099077542016 @default.
• W2009907754 countsByYear W20099077542017 @default.
• W2009907754 countsByYear W20099077542018 @default.
• W2009907754 countsByYear W20099077542019 @default.
• W2009907754 countsByYear W20099077542020 @default.
• W2009907754 countsByYear W20099077542021 @default.
• W2009907754 countsByYear W20099077542022 @default.
• W2009907754 crossrefType "journal-article" @default.
• W2009907754 hasAuthorship W2009907754A5013850715 @default.
• W2009907754 hasAuthorship W2009907754A5029252935 @default.
• W2009907754 hasAuthorship W2009907754A5033413143 @default.
• W2009907754 hasAuthorship W2009907754A5037093217 @default.
• W2009907754 hasAuthorship W2009907754A5042130936 @default.
• W2009907754 hasAuthorship W2009907754A5065419027 @default.
• W2009907754 hasAuthorship W2009907754A5069538040 @default.
• W2009907754 hasAuthorship W2009907754A5073070877 @default.

• next