NDLI: Nine non-symmetric pyrazine -pyridine imide-based complexes: reversible redox and isolation of $[M^{II/III}(pypzca)_{2}]^{0/+}$ when M = Co, Fe

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Nine non-symmetric pyrazine -pyridine imide-based complexes: reversible redox and isolation of $[M^{II/III}(pypzca)_{2}]^{0/+}$ when M = Co, Fe

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Cowan, Matthew G. Brooker, Sally
Description	Author Affiliation: Cowan MG ( Department of Chemistry and the MacDiarmid Institute for Advanced Materials and Nanotechnology, University of Otago, PO Box 56, Dunedin, 9054, New Zealand.)
Abstract	The non-symmetric imide ligand Hpypzca (N-(2-pyrazylcarbonyl)-2-pyridinecarboxamide) has been deliberately synthesised and used to produce nine first row transition metal complexes: $[M^{II}(pypzca)_{2}],$ M = Zn, Cu, Ni, Co, Fe; $[M^{III}(pypzca)_{2}]Y,$ M = Co and Y = $BF_{4},$ M = Fe and Y = $ClO_{4};$ $[Cu^{II}(pypzca)(H_{2}O)_{2}]BF_{4},$ $[Mn^{II}(pypzca)(Cl)_{2}]HNEt_{3}.$ These are the first deliberately prepared complexes of a non-symmetric imide ligand . X-ray crystal structures of $[Cu^{II}(pypzca)_{2}]·H_{2}O,$ $[Co^{II}(pypzca)_{2}],$ $[Co^{III}(pypzca)_{2}]BF_{4},$ $[Cu^{II}(pypzca)(H_{2}O)_{2}]BF_{4}·H_{2}O$ and $[Mn^{II}(pypzca)Cl_{2}]HNEt_{3}$ show that each of the $(pypzca)^{−}$ ligands binds in a meridional fashion via the $N_{3}$ donors. In the first three complexes, two such ligands are bound such that the ‘spare’ pyrazine nitrogen atoms are positioned approximately orthogonally to one another and also to the imide oxygen atoms. In MeCN the $[M^{II/III}(pypzca)_{2}]^{0/+}$ complexes, where M = Ni, Co or Fe, exhibit one reversible metal based $M^{II/III}$ process and two distinct, quasi-reversible ligand based reduction processes, the latter also observed for $M^{II}$ = Zn. $[Mn^{II}(pypzca)Cl_{2}]HNEt_{3}$ displays a quasi-reversible oxidation process in MeCN, along with several irreversible processes. Both copper(II) complexes show only irreversible processes. Variable temperature magnetic measurements show that $[Fe^{III}(pypzca)_{2}]ClO_{4}$ undergoes a gradual spin crossover from partially high spin at 298 K (3.00 BM) to fully low spin at 2 K (1.96 BM), and that $[Co^{II}(pypzca)_{2}]$ remains high spin from 298 to 4 K. All of the complexes are weakly coloured, other than $[Fe^{II}(pypzca)_{2}]$ which is dark purple and absorbs strongly in the visible region.
ISSN	14779226
Issue Number	5
Journal	Dalton Trans.
Volume Number	41
e-ISSN	13645447
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2012-02-07
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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