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Enisa Selimović Tatjana Vulović Biljana Petrović Živadin D. Bugarčić Jovana Bogojeski 《Transition Metal Chemistry》2013,38(6):635-640
The kinetics of the complex formation reactions of two [(TL tBu)PtCl]+ and [Pt(tpdm)Cl]+ complexes (TL tBu = 2,6-bis[(1,3-di-tert-butylimidazolin-2-imino)methyl]pyridine and tpdm = terpyridinedimethane) with N-donor ligands, l-histidine (L-His), inosine (Ino), inosine-5′-monophosphate (5′-IMP) and guanosine-5′-monophosphate (5′-GMP), were studied. All reactions were studied under pseudo-first-order conditions as a function of nucleophile concentration and temperature in aqueous 0.1 M NaClO4 solution in the presence of 10 mM NaCl using variable-temperature Uv–Vis spectrophotometry. The order of reactivity of the studied ligands is L-His > Ino > 5′-GMP > 5′-IMP. This order of reactivity is in relation to their electronic properties and structures. The mechanism of the substitution reactions is associative in nature as supported by the negative entropy of activation. 相似文献
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The Substitution Reactions of the Small Biomolecules and Dinuclear Pt(II) Complexes with Alkanediamine Linker
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The substitution reactions of the complexes [{trans‐Pt(NH3)2H2O}2(μ‐1,4‐diaminobutane)]4+ ( I ), [{trans‐Pt(NH3)2H2O}2(μ‐1,6‐diaminohexane)]4+ ( II ), and [{trans‐Pt(NH3)2H2O}2(μ‐1,8‐diaminooctane)]4+ ( III ), with nucleophiles L‐cysteine (L‐Cys), glutathione (GSH), guanosine‐5′‐monophosphate (5′‐GMP), L‐histidine (L‐His), and pyridine were studied in 0.1 M NaClO4 aqueous solutions at pH = 2.5. The substitutions were studied under pseudo‐first‐order conditions as a function of concentration and temperature using UV–vis spectrophotometry. At three different temperatures (288, 298, and 308 K) the reactions of the II and III complexes and 5′‐GMP were studied. The order of reactivity of study ligands is L‐Cys > GSH > 5′‐GMP > L‐His > pyridine and the order of reactivity of the complexes is I < II ≈ III . The obtained results indicate that the structure of the alkanediamine linker in the dinuclear Pt(II) complexes controls the substitution process. The negative values reported for entropy of activation confirmed the associative substitution mode. These results are discussed in order to find the connection between structure and reactivity of the dinuclear Pt(II) complexes. 相似文献
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Snežana Jovanović Jovana Bogojeski Marijana Petković 《Journal of Coordination Chemistry》2015,68(17-18):3148-3163
Substitution reactions of the dinuclear Pt(II) complexes, [{Pt(en)Cl}2(μ-pz)]2+ (1), [{Pt(dach)Cl}2(μ-pz)]2+ (2) and [{Pt(dach)Cl}2(μ-4,4?-bipy)]2+ (3), and corresponding aqua analogs with selected biologically important ligands, viz. 1,2,4-triazole, L-histidine (L-His) and guanosine-5?-monophosphate (5?-GMP) were studied under pseudo-first-order conditions as a function of concentration and temperature using UV–vis spectrophotometry. The reactions of the chloride complexes were followed in aqueous 25 mmol L?1 Hepes buffer in the presence of 40 mmol L?1 NaCl at pH 7.2, whereas the reactions of the aqua complexes were studied at pH 2.5. Two consecutive reaction steps, which both depend on the nucleophile concentration, were observed in all cases. The second-order rate constants for both reaction steps indicate a decrease in the order 1 > 2 > 3 for all complexes. Also, the pKa values of all three aqua complexes were determined. The order of the reactivity of the studied ligands is 1,2,4-triazole > L-His > 5?-GMP. 1H NMR spectroscopy and HPLC were used to follow the substitution of chloride in the dichloride 1, 2, and 3 complexes by guanosine-5?-monophosphate (5?-GMP). This study shows that the inert and bridging ligands have an important influence on the reactivity of the studied complexes. 相似文献
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Substitution reactions of the complexes [Pt(bpma)H2O]2+ and [PtCl(bpma)]+, where bpma is bis-(2-pyridylmethyl)amine, with the nitrogen-donor ligands 1,2,4-triazole, pyrazole and pyridazine were studied in aqueous 0.1 M
NaClO4 using variable-temperature UV–VIS spectrophotometry. The reactions of the aqua complex were studied at pH 2.5, and those
of the chloro complex were studied in the presence of 10 mM NaCl to prevent their hydrolysis. The values obtained for the
second-order rate constants indicate that the complexes with bpma are more reactive than those with diethylenetriamine. In
both cases, the aqua complexes are more reactive than the corresponding chloro complexes. The reactivity of the incoming ligands
follows the order: 1,2,4-triazole > pyridazine > pyrazole. Activation parameters were determined for all the reactions, and
the negative entropies of activation (∆S≠) support an A or Ia mechanism. 相似文献
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Bukonjić Andriana M. Tomović Dušan Lj. Stanković Ana S. Jevtić Verica V. Ratković Zoran R. Bogojeski Jovana V. Milovanović Jelena Z. Đorđević Dragana B. Arsenijević Aleksandar N. Milovanović Marija Z. Potočňák Ivan Trifunović Srećko R. Radić Gordana P. 《Transition Metal Chemistry》2019,44(1):65-76
Transition Metal Chemistry - Two copper(II) complexes with ligands derived from β-amino acids, 2-(1-aminocyclohexyl)acetic acid L1 and 2-(1-amino-4-(tert-butyl)cyclohexyl)acetic acid L2, were... 相似文献
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Dušan Lj. Tomović Andriana M. Bukonjić Verica V. Jevtić Zoran R. Ratković Jovana V. Bogojeski Ana Đeković Ivana D. Radojević Ljiljana R. Čomić Slađana B. Novaković Goran A. Bogdanović Srećko R. Trifunović Gordana P. Radić Snežana Cupara 《Transition Metal Chemistry》2018,43(2):137-148
The biological activities of two binuclear copper(II) complexes containing S-alkenyl derivatives of thiosalicylic acid are reported [alkenyl = propenyl (L1), isobutenyl (L2)]. The structure of the complex with the S-isobutenyl derivative (C2) was confirmed by single-crystal X-ray structure analysis, which revealed that the structure consists of centrosymmetric, dinuclear complex molecules [Cu2(S-i-butenyl-thiosal)4(DMSO)2] containing two Cu(II) centers bridged by four S-isobutyl-thiosalicylate ligands in a paddle-wheel type structure. The Cu(II) atom is situated in a distorted square-pyramidal environment formed by carboxylate oxygen atoms in the basal plane and a DMSO ligand in the axial position. The reactivities of the complexes toward guanosine-5′-monophosphate (5′-GMP) were investigated. Complex C2 ([Cu2(S-i-butenyl-thiosal)4(H2O)2]) reacted more rapidly with 5′-GMP than complex C1. The interactions of complexes C1 and C2 with calf thymus DNA (CT-DNA) were examined by absorption (UV–Vis) and emission spectral studies (ethidium bromide displacement studies), revealing good DNA interaction abilities. The antimicrobial activities of the free ligands and their complexes were tested by microdilution method, and both minimal inhibitory and microbicidal concentrations were determined. All the tested substances demonstrated selective and moderate antibacterial activity on gram-positive bacteria, but low antibacterial activity on gram-negative bacteria. Also, the tested substances demonstrated low antifungal activity. 相似文献
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Bogojeski J Jelić R Petrović D Herdtweck E Jones PG Tamm M Bugarčić ŽD 《Dalton transactions (Cambridge, England : 2003)》2011,40(24):6515-6523
The kinetics and the mechanism of the substitution reactions of the complex [(TL(tBu))PdCl](+), where TL(tBu) is 2,6-bis[(1,3-di-tert-butylimidazolin-2-imino)methyl]pyridine, with nucleophiles (guanosine-5'-monophosphate (5'-GMP), l-Methionine (l-Met) and l-Histidine (l-His)) were studied using variable-temperature stopped-flow techniques in aqueous 0.1 M NaClO(4) with 10 mM NaCl at 298 K. The order of reactivity is: l-Met > 5'-GMP > l-His. The formation equilibria of [(BL(iPr))Pd(H(2)O)(2)](2+), where BL(iPr) is 1,2-bis(1,3diisopropyl-4,5-dimethylimidazolin-2-imino)ethane, and [(TL(tBu))Pd(H(2)O)](2+) with some biologically relevant ligands (l-Met, 5'-GMP and l-His) were also studied. The stoichiometry and stability constants of the newly formed complexes are reported, and the concentration distribution of the various complex species has been evaluated as a function of pH. Comparing the values of logβ(1,1,0) for 5'-GMP, l-His and l-Met complexes, the most stable complex is with 5'-GMP followed by l-His and l-Met for both complexes, [(BL(iPr))Pd(H(2)O)(2)](2+) and [(TL(tBu))Pd(H(2)O)](2+). The crystal structures of [(TL(tBu))PdCl]ClO(4) and [(BL(iPr))PdCl(2)] were determined by X-ray diffraction. The coordination geometries around the palladium atoms are distorted square-planar, with the Pd-N1 distance to the central nitrogen atom of the TL(tBu) ligand, 1.944(2) ?, being shorter than those to the other two nitrogen atoms of TL(tBu), viz. 2.034(3) and 2.038(2) ?. The BL(iPr) complex displays similar Pd-N distances of 2.031(2) and 2.047(2) ?. 相似文献
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