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Developing Photosensitizer-Cobaloxime Hybrids for Solar-Driven H2 Production in Aqueous Aerobic Conditions
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Activating a [FeFe] Hydrogenase Mimic for Hydrogen Evolution under Visible Light.

Philipp Buday1, Chizuru Kasahara1,2, Elisabeth Hofmeister3

  • 1Institute of Inorganic and Analytical Chemistry, Friedrich Schiller University Jena, Humboldtstraße 8, 07743, Jena, Germany.

Angewandte Chemie (International Ed. in English)
|February 18, 2022
PubMed
Summary

This study introduces a novel, metal-free photosensitizer-catalyst dyad for efficient hydrogen evolution using visible light. The designed system mimics natural enzymes and achieves a turnover number of approximately 210.

Keywords:
H2 ProductionOligothiopheneOperando EPR SpectroscopyPhotocatalysis[FeFe] Hydrogenase Mimics

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Area of Science:

  • Bioinorganic Chemistry
  • Photocatalysis
  • Materials Science

Background:

  • Natural [FeFe] hydrogenases are highly efficient catalysts for hydrogen production.
  • Precious metal-free catalysts are desirable for sustainable energy applications.
  • Developing artificial systems that mimic natural enzymes is a key research area.

Purpose of the Study:

  • To design and synthesize a compact, precious metal-free photosensitizer-catalyst dyad (PS-CAT).
  • To investigate the photocatalytic hydrogen evolution activity of the PS-CAT under visible light.
  • To elucidate the mechanism of action using spectroscopic and electrochemical methods.

Main Methods:

  • Synthesis of a π-conjugated oligothiophene-based photosensitizer-catalyst dyad.
  • Steady-state and time-resolved spectroscopy.
  • Electrochemical techniques and photocatalytic experiments.
  • Operando Electron Paramagnetic Resonance (EPR) spectroscopy.
  • Theoretical calculations.

Main Results:

  • The PS-CAT effectively drove photocatalytic hydrogen evolution under visible light.
  • Operando EPR spectroscopy identified an active [FeI Fe0 ] species.
  • Theoretical calculations supported the proposed active species.
  • A turnover number (TON) of approximately 210 was achieved.

Conclusions:

  • The designed precious metal-free PS-CAT is a promising system for visible light-driven hydrogen evolution.
  • The active [FeI Fe0 ] species plays a crucial role in the catalytic process.
  • This work provides a blueprint for developing artificial hydrogenase mimics.