期刊
CHEMISTRY-AN ASIAN JOURNAL
卷 7, 期 6, 页码 1394-1400出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.201101020
关键词
bioinorganic chemistry; biomimetic compounds; hydrogen; ligand effects; oxygen
资金
- World Premier International Research Center Initiative (WPI)
- Global COE
- G30 Program
- Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan [18065017, 19205009, 23655053]
- JST, Japan
- Grants-in-Aid for Scientific Research [23655053, 19205009] Funding Source: KAKEN
Herein, we report a [NiRu] biomimetic system for O2-tolerant [NiFe]hydrogenases and demonstrate that electron donation to the [NiRu] center can switch the system between the activation of H2 and O2 through simple ligand effects by using hexamethylbenzene and pentamethylcyclopentadienyl ligands, respectively. Furthermore, we present the synthesis and direct observations of a [NiRu]peroxo species, which was formed by the oxygenation of a Ni-SIa model [NiRu] complex, that we propose as a biomimetic analogue of O2-bound species (OBS) of O2-tolerant [NiFe]hydrogenases. The [NiRu]peroxo complex was fully characterized by X-ray analysis, X-ray photoelectron spectroscopy (XPS), mass spectrometry, and 1H NMR spectroscopy. The OBS analogue was capable of oxidizing p-hydroquinone and sodium borohydride to turn back into the Ni-SIa model complex.
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