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Three-Dimensional Network Polymeric Structure of (2-Amino-5 Ammoniopyridinium)[CuCl4 ]: Crystal Supramolecularity and Magnetic Properties Sondra Walha · Houcine Naïli · Samia Yahyaoui · Basem Fares Ali · Mark M. Turnbull · Tahar Mhiri · Seik Weng Ng

Received: 25 April 2012 / Accepted: 21 August 2012 / Published online: 9 September 2012 © Springer Science+Business Media, LLC 2012

Abstract A single crystal structure determination of the complex (C5 H9 N3 )CuCl4 [henceforth I] has been carried out. It crystallizes in the orthorhombic space group Cmca, with the cell parameters a = 6.7053(5) Å, b = 22.4171(19) Å, c = 13.4173(9) Å, V = 2016.8(3) Å3 , and Z = 8. In the complex, the anion is comprised of infinite zigzag chains of monochloro-bridged CuCl2− 4 units · · ·–CuCl3 –μ–Cl–CuCl3 –μ–Cl–CuCl3 –· · · surrounded by the pyridinium-ammonium cations. The Cu ions are fivecoordinate to chloride ions in a distorted square-pyramidal geometry with the zigzag chains formed by corner-sharing polyhedra. The Cu ion is located 0.151 Å above the basal plane. In the crystal, there are four intermolecular hydrogen bonding interactions, linking the CuCl chains to the cations to form a 2D-network. The resulting 2D-networks are further linked by aryl· · ·aryl (π · · · π) interactions within the cationic chains leading to a 3D-network. Variable tem-

Electronic supplementary material The online version of this article (doi:10.1007/s10948-012-1759-y) contains supplementary material, which is available to authorized users. S. Walha · H. Naïli () · S. Yahyaoui · T. Mhiri Laboratoire de l’Etat Solide, Département de Chimie, Faculté des Sciences de Sfax, BP1171, 3000 Sfax, Tunisie e-mail: [email protected] B.F. Ali Department of Chemistry, Al al-Bayt University, Mafraq 25113, Jordan M.M. Turnbull Carlson School of Chemistry and Biochemistry, Clark University, Worcester , MA 01610, USA S.W. Ng Chemistry Department, Faculty of Science, University of Malaya, 50603 Kuala Lumpur, Malaysia

perature magnetic susceptibility data were fit to a onedimensional S = 1/2 antiferromagnetic chain model yielding C = 0.44(1) emu-K/mol-Oe and J = −37(1) K. Keywords Crystal structure · Polymeric CuCl4 anion · N–H· · ·Cl–Cu interactions · π · · · π interactions · 1D-antiferromagnetic chain

1 Introduction Intensive study in crystal engineering techniques has led to the establishment of new strategies and tactics for the preparation of materials with specific structural, magnetic, conductive, optical, etc. properties [1–4]. Considerable effort has been devoted to compounds of the general formula A2 MX4 where A is an organic cation, M is a divalent metal, and X is a halogen. Many of these compounds exhibit interesting magnetic properties which are related to the interhalide distances between the MX2− 4 anions, which are in turn strongly related to the properties of the organic cation [5–7]. The Cu(II) ion is an attractive transition metal ion for such studies because of its d9 configuration and single unpaired electron, making it an