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Efektywność grup donorowych nukleotydów w reakcjach z jonami metali w układach podwójnych i potrójnych z udziałem tetramin

Gąsowska A.

Wiadomości Chemiczne

2007

[Z] 61, 5-6

339-359

Nucleotides, being multifunctional ligands with donor nitrogen and oxygen atoms, take part in the majority of selective and specific processes occurring in nature [1-15]. It has been established that nucleotides react with the polyamines (biogenic amines) present in the living organisms and take part in genetic information transfer [16-24]. Nucleotides are composed of a purine or pyrimidine base, sugar residua and phosphate groups (Fig. 1) [25-27]. Each of the three components have potential centres of interaction with metal ions [28-29]. Because of the wide diversity of coordination possibilities there are often controversies as to the mode of coordination even in simple complexes with metal ions. Some authors claim that only nitrogen atoms of the nucleotide are effectively engaged in the metallation [30-43], while others maintain that it requires a combined engagement of nitrogen atoms and phosphate group [44-71]. There are also researchers who point to the involvement of only phosphate group of the nucleotide in the metallation [72-77]. The reaction of nucleotides with tetramines results in the formation of molecular complexes (Fig. 3) [78-88]. In the literature to date, there is no agreement as to the character of interactions and effectiveness of nucleotide donor groups in the formation of adducts with polyamines [80-82, 85-87, 89, 90]. According to some authors, the interaction between a nucleotide and polyamines in the metal-free systems has a noncovalent ion-ion or ion-dipole nature and the stability of molecular complexes is determined by the number of active centres in the reagents and the structural factor [80-84, 87]. According to other authors, it is a typical electrostatic interaction and the adduct stability is determined by the charge of the reagents [85, 89]. In the adducts formed by nucleotides with polyamines, the main interaction centres of a nucleotide are endocyclic nitrogen atoms and a phosphate group (the latter undergoes deprotonation already at a low pH), while in the case of tetramine the interaction centres are the NHx+ groups [77, 80-87, 89-91]. In the ternary systems of metal/nucleotide/tetramine, the following heteroligand molecular complexes are formed: MLźźźźźźHxL' (x = 4, HxL'-fully protonated polyamine) (Fig. 4) [80-82, 91, 94, 96], mixed protonated complexes MLHxL' (x = 1, 2, 3) (Fig. 5) [81, 82, 92, 96] and MLL' type complexes (Fig. 6) [81, 82, 91]. A significant influence of polyamines on the character of interactions of nucleotides with metal ions has been noted [80-82, 90-96]. In molecular complexes, the fully protonated polyamine is located in the outer coordination sphere. In the MLHxL' type complexes, the deprotonated nitrogen atoms of tetramine are involved in the coordination, while its protonated centres -NHx+ take part in noncovalent interactions that additionally stabilise the complex [81, 82, 92, 96, 97]. In the MLL' type complexes, oxygen atoms of nucleotide phosphate group and deprotonated nitrogen atoms of tetramine are in the inner coordination sphere, while nucleotide donor nitrogen atoms do not take part in the metallation [81, 82, 91].