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Photoinduced Hydrogen Evolution Catalyzed by Co(II) Complexes of N5-Donor Ligands

Li, Chuanshuai LU ; Li, Yong LU ; Luo, Yusen ; Michaliszyn, Klaudia ; Bolaño Losada, Iria LU ; Hossain, Md Kamal LU ; Elantabli, Fatma LU ; Guo, Meiyuan LU ; Hizbullah, Lintang LU and Tocher, Derek A. , et al. (2025) In Chemistry - A European Journal 31(28).
Abstract

Three new cobalt complexes of the general formula [Co(II)(L)(CH3CN)]2+, where L is one of three pentadentate nitrogen-donor ligands based on the N4Py framework, have been synthesized and characterized. The capacity of the three complexes to effect photocatalytic proton reduction has been examined. Their photocatalytic activities in the presence of [Ru(bpy)3]2+, acting as a photosensitizer, and ascorbic acid, acting as a sacrificial electron donor, were screened in a water/acetonitrile mixture. The photochemical mechanism, as revealed by nanosecond time-resolved transient absorption spectroscopy, involves reaction of the excited sensitizer with ascorbic acid to yield... (More)

Three new cobalt complexes of the general formula [Co(II)(L)(CH3CN)]2+, where L is one of three pentadentate nitrogen-donor ligands based on the N4Py framework, have been synthesized and characterized. The capacity of the three complexes to effect photocatalytic proton reduction has been examined. Their photocatalytic activities in the presence of [Ru(bpy)3]2+, acting as a photosensitizer, and ascorbic acid, acting as a sacrificial electron donor, were screened in a water/acetonitrile mixture. The photochemical mechanism, as revealed by nanosecond time-resolved transient absorption spectroscopy, involves reaction of the excited sensitizer with ascorbic acid to yield [Ru(bpy)3]+ as a primary photogenerated reductant, capable of electron transfer to the cobalt catalyst(s). Under the experimental conditions used, partial decomposition of both the sensitizer and the catalyst is the main deactivation channel for photocatalysis. Optimization of reaction conditions indicated that the use of more reducing iridium or copper-based photosensitizers had a beneficial effect on the catalytic performance. The effect of the different ligands on the catalytic activities of the corresponding cobalt complexes have been investigated by DFT calculations.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Co(II) complexes, Hydrogen evolution, N5-donor ligands, Photocatalysis
in
Chemistry - A European Journal
volume
31
issue
28
article number
e202404499
publisher
Wiley-Blackwell
external identifiers
  • scopus:105000675636
  • pmid:39982409
ISSN
0947-6539
DOI
10.1002/chem.202404499
language
English
LU publication?
yes
id
d66ff263-0a51-4828-bf1f-3dc8b02a136b
date added to LUP
2025-09-11 10:41:54
date last changed
2025-10-14 09:39:36
@article{d66ff263-0a51-4828-bf1f-3dc8b02a136b,
  abstract     = {{<p>Three new cobalt complexes of the general formula [Co(II)(L)(CH<sub>3</sub>CN)]<sup>2+</sup>, where L is one of three pentadentate nitrogen-donor ligands based on the N4Py framework, have been synthesized and characterized. The capacity of the three complexes to effect photocatalytic proton reduction has been examined. Their photocatalytic activities in the presence of [Ru(bpy)<sub>3</sub>]<sup>2+</sup>, acting as a photosensitizer, and ascorbic acid, acting as a sacrificial electron donor, were screened in a water/acetonitrile mixture. The photochemical mechanism, as revealed by nanosecond time-resolved transient absorption spectroscopy, involves reaction of the excited sensitizer with ascorbic acid to yield [Ru(bpy)<sub>3</sub>]<sup>+</sup> as a primary photogenerated reductant, capable of electron transfer to the cobalt catalyst(s). Under the experimental conditions used, partial decomposition of both the sensitizer and the catalyst is the main deactivation channel for photocatalysis. Optimization of reaction conditions indicated that the use of more reducing iridium or copper-based photosensitizers had a beneficial effect on the catalytic performance. The effect of the different ligands on the catalytic activities of the corresponding cobalt complexes have been investigated by DFT calculations.</p>}},
  author       = {{Li, Chuanshuai and Li, Yong and Luo, Yusen and Michaliszyn, Klaudia and Bolaño Losada, Iria and Hossain, Md Kamal and Elantabli, Fatma and Guo, Meiyuan and Hizbullah, Lintang and Tocher, Derek A. and Haukka, Matti and Persson, Petter and Lloret-Fillol, Julio and Dietzek-Ivanšić, Benjamin and Nordlander, Ebbe}},
  issn         = {{0947-6539}},
  keywords     = {{Co(II) complexes; Hydrogen evolution; N5-donor ligands; Photocatalysis}},
  language     = {{eng}},
  number       = {{28}},
  publisher    = {{Wiley-Blackwell}},
  series       = {{Chemistry - A European Journal}},
  title        = {{Photoinduced Hydrogen Evolution Catalyzed by Co(II) Complexes of N5-Donor Ligands}},
  url          = {{http://dx.doi.org/10.1002/chem.202404499}},
  doi          = {{10.1002/chem.202404499}},
  volume       = {{31}},
  year         = {{2025}},
}