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The reduction of ruthenium(III) complexes with triazolopyrimidine ligands by ascorbic acid and mechanistic insight into their action in anticancer therapy.
Autorzy
Rok wydania
2019
Czasopismo
Numer woluminu
484
Strony
305-310
DOI
10.1016/j.ica.2018.09.051
Kolekcja
Język
Angielski
Typ publikacji
Artykuł
Kinetic studies of the reduction of two ruthenium(III) complexes, mer-[RuCl3(dmso)(H2O)(tmtp)]·2H2O (1) and mer,cis-[RuCl3(dbtp)2(dmso)] (2) (where dmso – dimethylsulfoxide, tmtp – 5,6,7-trimethyl-1,2,4-triazolo[1,5-a]pyrimidine and dbtp – 5,7-ditertbutyl-1,2,4-triazolo[1,5-a]pyrimidine), by ascorbic acid were performed as a function of antioxidant concentration in acetate buffer within the pH range of 2.9–5. The rapid reduction of the ruthenium(III) complexes (1) and (2) resulted in the formation of the mer-[RuCl3(dmso)(H2O)(tmtp)]− and mer,cis-[RuCl3(dbtp)2(dmso)]− ions and was followed by successive dissociation of the chloride ligands. The second-order rate constant (k1) for the reduction of the mer-[RuCl3(dmso)(H2O)(tmtp)]·2H2O complex and the first-order rate constant for the hydrolysis of its reduced form were found to be 134 ± 2 M−1 s−1 and (3.8 ± 0.9) × 10−2 s−1 at 25 °C and pH = 2.9, respectively. Similarly, the fast process assigned to the reduction of the mer,cis-[RuCl3(dbtp)2(dmso)] complex and the subsequent, slower process attributed to the hydrolysis of the cis-[RuCl3(dbtp)2(dmso)]− ion were characterized by rate constants of 145.5 ± 0.8 M−1 s−1 and (9 ± 2) × 10−3 s−1 at 25 °C and pH = 2.9, respectively. Obtained data indicated that the reduction of the ruthenium(III) complexes strongly depends on pH and accelerates with increasing pH. The kinetic data indicates that the redox process followed an inner-sphere electron-transfer mechanism at pH higher than 3.
Adres publiczny
http://dx.doi.org/10.1016/j.ica.2018.09.051
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