Electrocatalytic hydrogen production using[FeFe]-hydrogenase mimics based on tetracene derivatives

Motonori Watanabe, Kenta Goto, Takaaki Miyazaki, Masahiko Shibahara, Yuan Jay Chang, Tahsin J. Chow, Tatsumi Ishihara

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

The synthesis, structure, physical properties, and electrocatalytic hydrogen production of tetrathiatetracene ligand based[FeFe]-hydrogenase mimic molecules were investigated. By adjusting the amount of iron, mono- A nd bis-[FeFe] coordinated complexes 1 and 2 were synthesized. The structures of 1 and 2 were analysed by NMR, IR, and absorption spectroscopies, and cyclic voltammetry and DFT computational analysis. In the DFT electron density maps, the HOMOs and LUMOs were located at tetrathiatetracene units, indicating that these complexes retain mainly acene characteristics. When weak acid Et3NHBF4 was added to CH2Cl2 solutions of 1 or 2, the reduction potential of iron complexes was shifted to more positive values proportional to the concentration of acid. As the acid concentration increased, the current of the reduction wave also increased, indicating the occurrence of a catalytic proton reduction reaction. The bulk electrolysis reaction showed 65.8 TON for 1 and 52.8 TON for 2.

Original languageEnglish
Pages (from-to)13810-13815
Number of pages6
JournalNew Journal of Chemistry
Volume43
Issue number35
DOIs
Publication statusPublished - Jan 1 2019

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Materials Chemistry

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