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Direct Probing of Photoinduced Electron Transfer in a Self-Assembled Biomimetic [2Fe2S]-Hydrogenase Complex Using Ultrafast Vibrational Spectroscopy.

Overview of attention for article published in Inorganic Chemistry, April 2014
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About this Attention Score

  • Above-average Attention Score compared to outputs of the same age (62nd percentile)
  • High Attention Score compared to outputs of the same age and source (87th percentile)

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4 tweeters
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1 Facebook page

Citations

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24 Dimensions

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37 Mendeley
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Title
Direct Probing of Photoinduced Electron Transfer in a Self-Assembled Biomimetic [2Fe2S]-Hydrogenase Complex Using Ultrafast Vibrational Spectroscopy.
Published in
Inorganic Chemistry, April 2014
DOI 10.1021/ic500777d
Pubmed ID
Authors

Ping Li, Li P, Amirjalayer S, Hartl F, Lutz M, Bruin BD, Becker R, Woutersen S, Reek JN, Bhagwat, V M, Ramachandran, B V, Saeed Amirjalayer, František Hartl, Martin Lutz, Bas de Bruin, René Becker, Sander Woutersen, Joost N. H. Reek

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.

Twitter Demographics

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Mendeley readers

The data shown below were compiled from readership statistics for 37 Mendeley readers of this research output. Click here to see the associated Mendeley record.

Geographical breakdown

Country Count As %
Netherlands 3 8%
United Kingdom 1 3%
Germany 1 3%
Unknown 32 86%

Demographic breakdown

Readers by professional status Count As %
Student > Ph. D. Student 10 27%
Student > Master 9 24%
Researcher 7 19%
Unspecified 3 8%
Student > Postgraduate 2 5%
Other 6 16%
Readers by discipline Count As %
Chemistry 27 73%
Unspecified 4 11%
Physics and Astronomy 2 5%
Agricultural and Biological Sciences 2 5%
Medicine and Dentistry 1 3%
Other 1 3%

Attention Score in Context

This research output has an Altmetric Attention Score of 2. This is our high-level measure of the quality and quantity of online attention that it has received. This Attention Score, as well as the ranking and number of research outputs shown below, was calculated when the research output was last mentioned on 24 September 2014.
All research outputs
#3,263,832
of 7,406,773 outputs
Outputs from Inorganic Chemistry
#1,400
of 8,577 outputs
Outputs of similar age
#63,881
of 174,190 outputs
Outputs of similar age from Inorganic Chemistry
#35
of 323 outputs
Altmetric has tracked 7,406,773 research outputs across all sources so far. This one has received more attention than most of these and is in the 54th percentile.
So far Altmetric has tracked 8,577 research outputs from this source. They receive a mean Attention Score of 1.1. This one has done well, scoring higher than 82% of its peers.
Older research outputs will score higher simply because they've had more time to accumulate mentions. To account for age we can compare this Altmetric Attention Score to the 174,190 tracked outputs that were published within six weeks on either side of this one in any source. This one has gotten more attention than average, scoring higher than 62% of its contemporaries.
We're also able to compare this research output to 323 others from the same source and published within six weeks on either side of this one. This one has done well, scoring higher than 87% of its contemporaries.