A noble-metal-free system for photocatalytic hydrogen production from water

Esteban Mejía, Shu Ping Luo, Michael Karnahl, Aleksej Friedrich, Stefanie Tschierlei, Annette Enrica Surkus, Henrik Junge, Serafino Gladiali, Stefan Lochbrunner, Matthias Beller

Research output: Contribution to journalArticlepeer-review

155 Scopus citations

Abstract

A series of heteroleptic copper(I) complexes with bidentate PP and NN chelate ligands was prepared and successfully applied as photosensitizers in the light-driven production of hydrogen, by using [Fe3(CO)12] as a water-reduction catalyst (WRC). These systems efficiently reduces protons from water/THF/triethylamine mixtures, in which the amine serves as a sacrificial electron donor (SR). Turnover numbers (for H) up to 1330 were obtained with these fully noble-metal-free systems. The new complexes were electrochemically and photophysically characterized. They exhibited a correlation between the lifetimes of the MLCT excited state and their efficiency as photosensitizers in proton-reduction systems. Within these experiments, considerably long excited-state lifetimes of up to 54μs were observed. Quenching studies with the SR, in the presence and absence of the WRC, showed that intramolecular deactivation was more efficient in the former case, thus suggesting the predominance of an oxidative quenching pathway.

Original languageEnglish
Pages (from-to)15972-15978
Number of pages7
JournalChemistry - A European Journal
Volume19
Issue number47
DOIs
StatePublished - 18 Nov 2013
Externally publishedYes

Keywords

  • copper
  • homogeneous catalysis
  • hydrogen
  • photochemistry
  • sustainable chemistry

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