Death and rebirth: Photocatalytic hydrogen production by a self-organizing copper-iron system

Steffen Fischer, Dirk Hollmann, Stefanie Tschierlei, Michael Karnahl, Nils Rockstroh, Enrico Barsch, Patrick Schwarzbach, Shu Ping Luo, Henrik Junge, Matthias Beller, Stefan Lochbrunner, Ralf Ludwig, Angelika Brückner

Research output: Contribution to journalReview articlepeer-review

88 Scopus citations

Abstract

This study provides detailed mechanistic insights into light-driven hydrogen production using an abundant copper-iron system. It focuses on the role of the heteroleptic copper photosensitizer [Cu(PP)(N N)]+, which can be oxidized or reduced after photoexcitation. By means of IR, EPR, and UV/vis spectroscopy as well as computational studies and spectroelectrochemistry, the possibility of both mechanisms was confirmed. UV/vis spectroscopy revealed the reorganization of the original heteroleptic photosensitizer during catalysis toward a homoleptic [Cu(NN)2]+ species. Operando FTIR spectroscopy showed the formation of a catalytic diiron intermediate, which resembles well-known hydrogenase active site models.

Original languageEnglish
Pages (from-to)1845-1849
Number of pages5
JournalACS Catalysis
Volume4
Issue number6
DOIs
StatePublished - 6 Jun 2014
Externally publishedYes

Keywords

  • catalytic intermediates
  • copper photosensitizer
  • iron catalysts
  • operando spectroscopy
  • proton reduction

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