期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 2022, 期 3, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.202100959
关键词
Cyclic voltammetry; [FeFe] hydrogenase; Naphthalene monoimide; Quantum chemistry; Spectroelectrochemistry
资金
- German Science Foundation (DFG) [TRR234, 364549901]
- Projekt DEAL
Hydrogenase mimicking complexes with N-substituted naphthalene monoimide (NMI) of peri-substituted dichalcogenides as bridging ligands were prepared and characterized using various spectroscopic techniques. The redox behavior of these complexes was investigated through cyclic voltammetry, IR and UV-Vis spectroelectrochemistry, EPR spectroscopy and quantum chemical simulations. EPR experiments revealed the non-innocent character of the NMI bridging ligands, showing the formation of an organic radical and a dimeric structure after successive reductions.
[FeFe] hydrogenase mimicking complexes containing N-substituted naphthalene monoimide (NMI) of peri-substituted dichalcogenides as bridging ligands have been prepared and characterized using different spectroscopic as well as by X-ray diffraction methods. The redox behaviour has been investigated by cyclic voltammetry, IR and UV-Vis spectroelectrochemistry (IR and UV-Vis SEC), electron paramagnetic resonance (EPR) spectroscopy and quantum chemical simulations. IR SEC and EPR experiments combined with DFT calculations revealed the non-innocent character of the NMI bridging ligands. EPR spectroscopy was applied to study the singly and doubly reduced state. Chemical reduction with one equivalent of Cp*Co-2 revealed the formation of an organic radical with a g-value of 2.0028 at room temperature. When two equivalents of Cp*Co-2 were used to carry out the second reduction, no EPR signal could be detected anymore. IR SEC measurements indicate the formation of an EPR-silent dimeric structure after the second reduction.
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