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

研究成果: ジャーナルへの寄稿記事

抄録

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.

元の言語英語
ページ(範囲)13810-13815
ページ数6
ジャーナルNew Journal of Chemistry
43
発行部数35
DOI
出版物ステータス出版済み - 1 1 2019

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Hydrogenase
Hydrogen production
Derivatives
Discrete Fourier transforms
Acids
Iron
Absorption spectroscopy
Electrolysis
Nuclear magnetic resonance spectroscopy
Cyclic voltammetry
Carrier concentration
Protons
Infrared spectroscopy
Physical properties
Ligands
Molecules
naphthacene

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Materials Chemistry

これを引用

Electrocatalytic hydrogen production using[FeFe]-hydrogenase mimics based on tetracene derivatives. / Watanabe, Motonori; Goto, Kenta; Miyazaki, Takaaki; Shibahara, Masahiko; Chang, Yuan Jay; Chow, Tahsin J.; Ishihara, Tatsumi.

:: New Journal of Chemistry, 巻 43, 番号 35, 01.01.2019, p. 13810-13815.

研究成果: ジャーナルへの寄稿記事

Watanabe, Motonori ; Goto, Kenta ; Miyazaki, Takaaki ; Shibahara, Masahiko ; Chang, Yuan Jay ; Chow, Tahsin J. ; Ishihara, Tatsumi. / Electrocatalytic hydrogen production using[FeFe]-hydrogenase mimics based on tetracene derivatives. :: New Journal of Chemistry. 2019 ; 巻 43, 番号 35. pp. 13810-13815.
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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.",
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AU - Watanabe, Motonori

AU - Goto, Kenta

AU - Miyazaki, Takaaki

AU - Shibahara, Masahiko

AU - Chang, Yuan Jay

AU - Chow, Tahsin J.

AU - Ishihara, Tatsumi

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AB - 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.

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