Polyhedron 20 (2001) 3239 – 3247 Synthesis of cobalt(II) complexes of derivatised salicylaldoxime ligands; X-ray crystal structures of DMSO adducts of bis(3-nitro-5-methylsalicylaldoximato)cobalt(II) and bis(3-nitro-5-phenylsalicylaldoximato)cobalt(II) Domenico Cupertino a , Mary McPartlin b , Andreas M. Zissimos b, * a AVECIA, Hexagon House, Blackley, Manchester M98ZS, UK b School of Biological and Applied Sciences, Uniersity of North London, 166 -220 Holloway Road, London N78DP, UK Received 11 July 2001; accepted 24 September 2001 Abstract A total of five salicylaldoxime ligands, (HL 1–5 ), analogues of commercial metal extractants were synthesised and characterised. The cobalt(II) complexes [CoL 2 ] (L =L 1–5 ) of these ligands were synthesised and characterised by microanalysis, atomic absorption, infra and mass spectroscopy. X-ray structure analysis was carried out on the adducts [Co(L) 2 (dmso) 2 ] (L =L 4,5 ). These are the only structurally characterised cobalt salicylaldoxime complexes apart from three five-coordinate nitroso complexes [CoL 2 (NO)] reported in the 1980s (J. Crystallogr. Spectrosc. Res. 13 (1983) 413; J. Crystallogr. Spectrosc. Res. 16 (1986) 6). The structures of the two adducts characterised show octahedral coordination with two dmso molecules occupying axial positions and two salicylaldoxime units in each molecule occupying equatorial positions. The introduction of nitro groups on the two ligands has been found to stabilise oxidation (II) in preference to (III) in both cobalt complexes. These groups were found to have what appears to be a significant contribution to intra-ligand hydrogen bonding resulting in three-centre H bonds on either side of the molecules, which in turn adopt unusual chair conformations. © 2001 Elsevier Science Ltd. All rights reserved. Keywords: Salicylaldoxime ligands; Cobalt(II) complexes; X-ray crystal structures; DMSO adducts www.elsevier.com/locate/poly 1. Introduction Early work on the extractive properties of salicylal- doximes had established them as very good extractants for copper [3 – 5] and various extractants were devel- oped based on these ligands [6]. Attempts, however, to use these compounds in the extraction of cobalt [7] failed for a number of reasons, but much of this work has been carried out in industrial laboratories and has not been well documented in the general scientific liter- ature. In 1975, Ashbrook [8], in a review on chelating reagents in solvent extraction, discussed the problem involved in the extraction of cobalt using these ligands. When cobalt was extracted from solutions at pH 7–9, by salicylaldoxime-based extractants, it was found to be very difficult to strip (i.e. to be separated from the ligand used in the extraction process by acidification of the complex); even concentrated acids had little effect on the extracted complex. This was generally assumed to be the result of oxidation of Co(II) to Co(III), with the formation of very stable Co(III) salicylaldoxime complexes in the solvent phase. The absence of any structural data on the square planar bis chelate cobalt(II) complexes of salicylal- doxime ligands, apart from 3 five coordinate nitroso complexes [CoL 2 (NO)] reported in the 1980’s [1,2], and the need to develop new derivatives of these ligands that might stabilise cobalt in oxidation state (II) upon complexation has motivated the present work. It was thought, that steric hindrance introduced on the ligands in the form of bulky substituents R 1 and R 2 , would * Corresponding author. Present address: Chemistry Department, University College London, 20 Gordon Street, London WC1H 0AJ, UK. Tel.: +44-207-679-4639; fax: +44-207-679-4603. E-mail address: a.zissimos@ucl.ac.uk (A.M. Zissimos). 0277-5387/01/$ - see front matter © 2001 Elsevier Science Ltd. All rights reserved. PII:S0277-5387(01)00947-0