One- versus two-electron oxidation of complexed guanidino-functionalized aromatic compounds
Herein, we report a rational synthetic access to dinuclear CuII complexes with radical monocationic guanidine ligands. The starting point was the first directed synthesis of a dinuclear CuII complex of the redox-active, neutral guanidino-functionalized aromatic (GFA) compound 1,2,4,5-tetrakis(tetram...
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| Main Authors: | , , , , , , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
06 November 2014
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| In: |
European journal of inorganic chemistry
Year: 2014, Issue: 35, Pages: 6039-6050 |
| ISSN: | 1099-0682 |
| DOI: | 10.1002/ejic.201402840 |
| Online Access: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1002/ejic.201402840 Verlag, lizenzpflichtig, Volltext: https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/ejic.201402840 
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| Author Notes: | Christine Trumm, Olaf Hübner, Petra Walter, Simone Leingang, Ute Wild, Elisabeth Kaifer, Benjamin Eberle, and Hans-Jörg Himmel |
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| 245 | 1 | 0 | |a One- versus two-electron oxidation of complexed guanidino-functionalized aromatic compounds |c Christine Trumm, Olaf Hübner, Petra Walter, Simone Leingang, Ute Wild, Elisabeth Kaifer, Benjamin Eberle, and Hans-Jörg Himmel |
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| 520 | |a Herein, we report a rational synthetic access to dinuclear CuII complexes with radical monocationic guanidine ligands. The starting point was the first directed synthesis of a dinuclear CuII complex of the redox-active, neutral guanidino-functionalized aromatic (GFA) compound 1,2,4,5-tetrakis(tetramethylguanidino)benzene (1) as ligand by treatment of 1 with Cu(OAc)2. The neutral complex [1Cu(OAc)22] was then oxidized with several oxidizing reagents. With I2 two-electron oxidation occurred, thus leading to green salts of the dication [1Cu(OAc)22]2+. In contrast, with AgPF6 or AgSbF6 one-electron oxidation was observed to yield red salts of the monocation [1Cu(OAc)22]+, which is a three-spin system with one unpaired electron at each copper atom and at the ligand unit. Superconducting quantum interference device (SQUID) magnetometric measurements confirm a quartet electronic ground state that arises from strong ferromagnetic copper-ligand coupling. Intense charge-transfer transitions in the visible region (576 and 536 nm) were observed in the electronic absorption spectra and assigned to strong ligand-ligand (1·+←OAc) charge-transfer (LLCT) excitations. These LLCT bands open up the possibility of photoinduced redox reactions with [1Cu(OAc)22]+ driven by restoration of the aromatic system at the GFA ligand. | ||
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| 650 | 4 | |a Oxidation | |
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