Interactions of the "piano-stool" [ruthenium(II) (eta6-arene)(en)CL]+ complexes with water and nucleobases; ab initio and DFT study

Interactions of the "piano-stool" [ruthenium(II) (eta6-arene)(en)CL]+ complexes with water and nucleobases; ab initio and DFT study

Copyright 2008 Wiley Periodicals, Inc.

Détails bibliographiques
Publié dans:Journal of computational chemistry. - 1984. - 30(2009), 12 vom: 15. Sept., Seite 1758-70
Auteur principal: Futera, Zdenek (Auteur)
Autres auteurs: Klenko, Julia, Sponer, Judit E, Sponer, Jirí, Burda, Jaroslav V
Format: Article en ligne
Langue:English
Publié: 2009
Accès à la collection:Journal of computational chemistry
Sujets:Journal Article Research Support, Non-U.S. Gov't Antineoplastic Agents Ethylenediamines Purines Pyrimidinones Water 059QF0KO0R Uracil 56HH86ZVCT plus... Guanine 5Z93L87A1R ethylenediamine 60V9STC53F Ruthenium 7UI0TKC3U5 Cytosine 8J337D1HZY Adenine JAC85A2161 Thymine QR26YLT7LT
LEADER 01000caa a22002652 4500
001 NLM185250432
003 DE-627
005 20250210010335.0
007 cr uuu---uuuuu
008 231223s2009 xx |||||o 00| ||eng c
024 7 |a 10.1002/jcc.21179  |2 doi 
028 5 2 |a pubmed25n0618.xml 
035 |a (DE-627)NLM185250432 
035 |a (NLM)19090568 
040 |a DE-627  |b ger  |c DE-627  |e rakwb 
041 |a eng 
100 1 |a Futera, Zdenek  |e verfasserin  |4 aut 
245 1 0 |a Interactions of the "piano-stool" [ruthenium(II) (eta6-arene)(en)CL]+ complexes with water and nucleobases; ab initio and DFT study 
264 1 |c 2009 
336 |a Text  |b txt  |2 rdacontent 
337 |a ƒaComputermedien  |b c  |2 rdamedia 
338 |a ƒa Online-Ressource  |b cr  |2 rdacarrier 
500 |a Date Completed 02.11.2009 
500 |a Date Revised 20.11.2014 
500 |a published: Print 
500 |a Citation Status MEDLINE 
520 |a Copyright 2008 Wiley Periodicals, Inc. 
520 |a Piano stool ruthenium complexes of the composition [Ru(II)(eta6-arene)(en)Cl](+/2+) (en = ethylenediamine) represent an emerging class of cisplatin-analogue anticancer drug candidates. In this study, we use computational quantum chemistry to characterize the structure, stability and reactivity of these compounds. All these structures were optimized at DFT(B3LYP)/6-31G(d) level and their single point properties were determined by the MP2/6-31++G(2df,2pd) method. Thermodynamic parameters and rate constants were determined for the aquation process, as a replacement of the initial chloro ligand by water and subsequent exchange reaction of aqua ligand by nucleobases. The computations were carried out at several levels of DFT and ab initio theories (B3LYP, MP2 and CCSD) utilizing a range of bases sets (from 6-31G(d) to aug-cc-pVQZ). Excellent agreement with experimental results for aquation process was obtained at the CCSD level and reasonable match was achieved also with the B3LYP/6-31++G(2df,2pd) method. This level was used also for nucleobase-water exchange reaction where a smaller rate constant for guanine exchange was found in comparison with adenine. Although adenine follows a simple replacement mechanism, guanine complex passes by a two-step mechanism. At first, Ru-O6(G) adduct is formed, which is transformed through a chelate TS2 to the Ru-N7(G) final complex. In case of guanine, the exchange reaction is more favorable thermodynamically (releasing in total by about 8 kcal/mol) but according to our results, the rate constant for guanine substitution is slightly smaller than the analogous constant in adenine case when reaction course from local minimum is considered 
650 4 |a Journal Article 
650 4 |a Research Support, Non-U.S. Gov't 
650 7 |a Antineoplastic Agents  |2 NLM 
650 7 |a Ethylenediamines  |2 NLM 
650 7 |a Purines  |2 NLM 
650 7 |a Pyrimidinones  |2 NLM 
650 7 |a Water  |2 NLM 
650 7 |a 059QF0KO0R  |2 NLM 
650 7 |a Uracil  |2 NLM 
650 7 |a 56HH86ZVCT  |2 NLM 
650 7 |a Guanine  |2 NLM 
650 7 |a 5Z93L87A1R  |2 NLM 
650 7 |a ethylenediamine  |2 NLM 
650 7 |a 60V9STC53F  |2 NLM 
650 7 |a Ruthenium  |2 NLM 
650 7 |a 7UI0TKC3U5  |2 NLM 
650 7 |a Cytosine  |2 NLM 
650 7 |a 8J337D1HZY  |2 NLM 
650 7 |a Adenine  |2 NLM 
650 7 |a JAC85A2161  |2 NLM 
650 7 |a Thymine  |2 NLM 
650 7 |a QR26YLT7LT  |2 NLM 
700 1 |a Klenko, Julia  |e verfasserin  |4 aut 
700 1 |a Sponer, Judit E  |e verfasserin  |4 aut 
700 1 |a Sponer, Jirí  |e verfasserin  |4 aut 
700 1 |a Burda, Jaroslav V  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Journal of computational chemistry  |d 1984  |g 30(2009), 12 vom: 15. Sept., Seite 1758-70  |w (DE-627)NLM098138448  |x 1096-987X  |7 nnns 
773 1 8 |g volume:30  |g year:2009  |g number:12  |g day:15  |g month:09  |g pages:1758-70 
856 4 0 |u http://dx.doi.org/10.1002/jcc.21179  |3 Volltext 
912 |a GBV_USEFLAG_A 
912 |a SYSFLAG_A 
912 |a GBV_NLM 
912 |a GBV_ILN_350 
951 |a AR 
952 |d 30  |j 2009  |e 12  |b 15  |c 09  |h 1758-70