NDLI: Flipping of the coordinated triazine moiety in $Cu(I)–L_{2}$ and the small electronic factor, $κ_{el},$ for direct outer-sphere cross reactions: syntheses, crystal structures and redox behaviour of $copper(II)/(I)–L_{2}$ complexes (L = 3-(2-pyridyl)-5,6-diphenyl-1,2,4-triazine)

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Flipping of the coordinated triazine moiety in $Cu(I)–L_{2}$ and the small electronic factor, $κ_{el},$ for direct outer-sphere cross reactions: syntheses, crystal structures and redox behaviour of $copper(II)/(I)–L_{2}$ complexes (L = 3-(2-pyridyl)-5,6-diphenyl-1,2,4-triazine)

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Flipping of the coordinated triazine moiety in $Cu(I)–L_{2}$ and the small electronic factor, $κ_{el},$ for direct outer-sphere cross reactions: syntheses, crystal structures and redox behaviour of $copper(II)/(I)–L_{2}$ complexes (L = 3-(2-pyridyl)-5,6-diphenyl-1,2,4-triazine)

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Inamo, Masahiko Takagi, Hideo D. Yamada, Atsutoshi Suzuki, Takayoshi Yamane, Ryohei Mabe, Takuya Noda, Kyoko Wasada, Yuko Ishihara, Koji
Description	Author Affiliation: Yamada A ( Research Center for Materials Science, Nagoya University, Nagoya 464-8602, Japan. h.d.takagi@nagoya-u.jp.)
Abstract	Six-coordinate $[Cu(pdt)_{2}(H_{2}O)_{2}]^{2+}$ and four-coordinate $[Cu(pdt)_{2}]^{+}$ complexes were synthesized and the cross redox reactions were studied in acetonitrile (pdt = 3-(2-pyridyl)-5,6-diphenyl-1,2,4-triazine). Single crystal analyses revealed that $[Cu(pdt)_{2}(H_{2}O)_{2}](BF_{4})_{2}$ was of $pseudo-D_{2h}$ symmetry with two axial water molecules and two symmetrically coordinated equatorial pdt ligands, while the coordination structure of $[Cu(pdt)_{2}]BF_{4}$ was a squashed tetrahedron (dihedral angle = 54.87°) with an asymmetric coordination by two pdt ligands: one pdt ligand was coordinated to Cu(I) through pyridine-N and triazine-N2 while another pdt ligand was coordinated through pyridine-N and triazine-N4, and a stacking interaction between the phenyl ring on one pdt ligand and the triazine ring on another pdt ligand caused the squashed structure and non-equivalent Cu–N bond lengths. The cyclic voltammograms for $[Cu(pdt)_{2}(H_{2}O)_{2}]^{2+}$ and $[Cu(pdt)_{2}]^{+}$ in acetonitrile were identical to each other and quasi-reversible. The reduction of $[Cu(pdt)_{2}(H_{2}O)_{2}]^{2+}$ by decamethylferrocene and the oxidation of $[Cu(pdt)_{2}]^{+}$ by $[Co(2,2′-bipyridine)_{3}]^{3+}$ in acetonitrile revealed that both cross reactions were sluggish through a gated process (the structural change took place prior to the electron transfer) accompanied by slow direct electron transfer processes. It was found that the triazine ring of the coordinated pdt ligand rotates around the C–C bond between the triazine and pyridine rings with the kinetic parameters k = 51 ± 5 $s^{−1}$ (297.8 K), $ΔH^{‡}$ = 6.2 ± 1.1 kJ $mol^{−1}$ and $ΔS^{‡}$ = −192 ± 4 J $mol^{−1}$ $K^{−1}.$ The electron self-exchange process was directly measured using the line-broadening method: $k_{ex}$ = (9.9 ± 0.5) × $10^{4}$ kg $mol^{−1}$ $s^{−1}$ (297.8 K) with $ΔH^{‡}$ = 44 ± 7 kJ $mol^{−1}$ and $ΔS^{‡}$ = 0.2 ± 2.6 J $mol^{−1}$ $K^{−1}.$ By comparing this rate constant with the self-exchange rate constants estimated from the cross reactions using the Marcus cross relation, the non-adiabaticity (electronic) factors, $κ_{el},$ for the direct electron transfer processes between $[Cu(pdt)_{2}]^{+/2+}$ and non-copper metal $(Fe^{2+}$ and $Co^{3+})$ complexes were estimated as ca. $10^{−7},$ indicating that the electronic coupling between the d orbitals of copper and of non-copper metals is very small.
ISSN	14779226
Issue Number	31
Journal	Dalton Trans.
Volume Number	44
e-ISSN	13645447
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2015-08-21
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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