TY - JOUR
T1 - Electrocatalytic hydrogen production using[FeFe]-hydrogenase mimics based on tetracene derivatives
AU - Watanabe, Motonori
AU - Goto, Kenta
AU - Miyazaki, Takaaki
AU - Shibahara, Masahiko
AU - Chang, Yuan Jay
AU - Chow, Tahsin J.
AU - Ishihara, Tatsumi
N1 - Funding Information:
This work was supported by a Grant-in-Aid for Science Research (JP17H04888, JP17K19123) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), and Japan and the Strategic International Collaborative Research Program (SICORP) in ‘‘Research on Hydrogen as a renewable energy carrier’’ from Japan Science and Technology Agency (JST), Japan, and was performed under the Cooperative Research Program of ‘‘Network Joint Research Centre for Materials and Devices’’ (IMCE, Kyushu University). YJC and TJC acknowledge support from the Ministry of Science and Technology, Taiwan (MOST 107-2113-M-029-010-). MW acknowledges support from I2CNER, funded by the World Premier International Research Centre Initiative (WPI), Ministry of Education, Culture, Sports, Science and Technology of Japan (MEXT), Japan.
Publisher Copyright:
© 2019 The Royal Society of Chemistry and the Centre National de la Recherche Scientifique.
PY - 2019
Y1 - 2019
N2 - 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.
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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U2 - 10.1039/c9nj02790d
DO - 10.1039/c9nj02790d
M3 - Article
AN - SCOPUS:85072166271
SN - 1144-0546
VL - 43
SP - 13810
EP - 13815
JO - New Journal of Chemistry
JF - New Journal of Chemistry
IS - 35
ER -
