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Keywords:

  • electron transfer;
  • hydrogen;
  • iron;
  • photochemistry;
  • sensitizers

Abstract

To mimic [FeFe] hydrogenases (H2ases) in nature, molecular photocatalysts 1a, 1b, and 1c anchoring rhenium(I) complex S to one of the iron cores of [FeFe]-H2ases model complex C, have been constructed for H2 generation by visible light in homogeneous solution. The time-dependence of H2 evolution and a spectroscopic study demonstrate that the orientation of S and the specific bridge in 1a, 1b, and 1c are important both for the electron-transfer step from the excited S* to the catalytic C, and the formation of unprecedented long-lived charge separation for 1a (780 μs), 1b, and 1c (>2 ms) in [FeFe]-H2ases mimics. The fast forward electron-transfer step from the excited S* to the catalytic C but the slow back electron-transfer step of the charge-recombination in the designed photocatalysts 1a, 1b, and 1c are reminiscent of the behavior of [FeFe]-H2ases in nature.

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Featured Compounds

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  1. 1 - 13
Compound 1a
Molecular Weight:1118.561
Molecular Formula:C39H24BrFe2N4O8ReS2
InChIKey:Not Available
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Compound 1b
Molecular Weight:1266.826
Molecular Formula:C45H30F3Fe2N5O11ReS3
InChIKey:GDYYUTPTAKIXAL-UHFFFAOYSA-K
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Compound 1c
Molecular Weight:1161.689
Molecular Formula:C38H23F3Fe2N4O11ReS3
InChIKey:RWDNYSFQBCNYLU-UHFFFAOYSA-K
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Compound 1d
Molecular Weight:461.072
Molecular Formula:C15H11Fe2NO5S2
InChIKey:Not Available
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Compound 2a
Molecular Weight:635.484
Molecular Formula:C22H15BrN3O3Re
InChIKey:Not Available
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Compound 2b
Molecular Weight:883.866
Molecular Formula:C36H25F3N4O6ReS
InChIKey:UBBNBSZLRNXOED-UHFFFAOYSA-M
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Compound 2c
Molecular Weight:778.729
Molecular Formula:C29H18F3N3O6ReS
InChIKey:OQKHFTDPPZQUCJ-UHFFFAOYSA-M
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Compound 3
Molecular Weight:586.968
Molecular Formula:C15H10Fe2INO5S2
InChIKey:Not Available
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Compound 4
Molecular Weight:562.177
Molecular Formula:C22H14Fe2N2O5S2
InChIKey:Not Available
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Compound 5
Molecular Weight:364.239
Molecular Formula:C19H14BrN3
InChIKey:Not Available
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Compound 6
Molecular Weight:309.3639
Molecular Formula:C21H15N3
InChIKey:Not Available
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Compound 7
Molecular Weight:768.42
Molecular Formula:C36H24Fe2N4O5S2
InChIKey:Not Available
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Compound 8
Molecular Weight:285.3425
Molecular Formula:C19H15N3
InChIKey:Not Available
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  1. 1 - 13