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Organic phosphonic acid and its metal complexes synthesis , structure and magnetic properties of

Author: DingDeGang
Tutor: LuHuiJie；WangMinCan
School: Zhengzhou University
Course: Organic Chemistry
Keywords: Phosphonates Synthesis Magnetic Properties Antiferromagnetic interaction Skeleton structure Polymer Trimer Magnetic Properties NH3 Layered structure
CLC: O641.4
Type: Master's thesis
Year: 2004
Downloads: 117
Quote: 1
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Abstract


In this thesis, nine organic phosphonic acid compounds have been prepared and characterized by IR and E.A. Two novel metal phosphonates with three-dimensional open framework structures namely Co3[CH3C(NH3)(PO3H)2]2[CH3C(NH3)(PO3)(PO3H )]2(H2O)4 (1) and Cu4[CH3C(NH2)(PO3)2]2(C10H8N2)(H2O)4 (2) were synthesized under hydrothermal conditions in which the phosphonic acid CH3C(NH3)(PO3H)2 [aedp] was used. The magnetic study indicates there is a antiferromagnetic exchange between the magnetic centers for each metal phosphonate.Single crystal structural determinations for polymer 1 reveals a three-dimensional open framework structure formed with {Co3[CH3C(NH3)(PO3H)2]2[CH3C(NH3)(PO3)(P O3H)]2(H2O)4}n layers, in which each layer is constructed by symmetric {Co3(aedp)4(H2O)4} trimer units. The Co(l)O6 octahedra and Co(2)O6 octahedra is fused by corner-sharing with CPO3 tetrahedra independently, forming a finite chain {CO3[CH3C(NH3)(PO3H)2]2[CH3C(NH3)(PO3)(PO3H)]2(H2O)4} along the c-axis direction. In each chain two CH3C(NH3)(PO3)(PO3H) ligands bridge Co(l) and Co(2) atom to form a {Co3(aedp)4(H2O)4} trimer unit, the neighboring trimers are connected together through 0(9) and 0(11) atoms coordinated to equivalent Co(l) atoms, leading to a two-dimensional layer of {Co3[CH3C(NH3)(PO3H)2]2[CH3C(NH3)(PO3)(PO3H)]2(H 20)4}n in approximately [011] direction. The O(9) and O(11) atoms behave as bridge to connect different layers also, the Co(1)O6 octahedra and Co(2)O6 octahedra from different layers are bridged by the means of corner-sharing with two CPO3 tetrahedra independently, as a result a stair-like structure is formed.OSThe structure of polymer 2 is composed of {Cu4(aedp)2(H2O)2}n layers connected by 4,4’-bipyridine bridges. Each aedp ligand group behaves as a bis(chelating) ligand to bridge Cu(1) and Cu(2) atoms, forming {Cu3(aedp)2} trimer units. The neighboring trimers are fused together by the coordination of the phosphonate oxygen O(2) to the equivalent Cu(1) atom, hence forming an infinite chain along the [ 0 0 1 ] direction with a ladder-like motif. These chains are connected through {Cu(3)O4} units by sharing the remaining phosphonate oxygen O(7) of aedp ligand. As a result a two-dimensional network structure of copper phosphonate is constructed in the ac plane. The layers are linked by 4.4’-bipyridine bridging ligands, thus forming a three-dimensional open framework structure.The magnetic studies of polymer 1 show a dominant antiferromagnetic exchange between the Co ions. The overall magnetic behavior is mainly attributed to the antiferromagnetic interaction between magnetic centers through O-P-O bridge considering the structure of polymer 1 in which composed of {{Co3[CH3C(NH3)(PO3H)2]2[CH3C(NH3)(PO3)(PO3H)]2(H2O)4}n layers connected by O atoms.The magnetic studies of polymer 2 also show a dominant antiferromagnetic exchange between the Cu ions. Theoretical fitting of the data in the temperature range 25-300K results in the parameters g=1.85, J=-75.89398, Na=0.00737. The negative J value confirms the presence of antiferromagnetic interactions.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Structural Chemistry > Complex chemistry ( coordination chemistry )
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