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Side Reactions with an Equilibrium Constraint: Detailed Mechanism of the Substitution Reaction of Tetraplatin with dGMP as a Starting Step of the Platinum(IV) Reduction Process

The result's identifiers

  • Result code in IS VaVaI

    <a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F17%3A10367400" target="_blank" >RIV/00216208:11320/17:10367400 - isvavai.cz</a>

  • Result on the web

    <a href="http://dx.doi.org/10.1021/acs.jpcb.7b01427" target="_blank" >http://dx.doi.org/10.1021/acs.jpcb.7b01427</a>

  • DOI - Digital Object Identifier

    <a href="http://dx.doi.org/10.1021/acs.jpcb.7b01427" target="_blank" >10.1021/acs.jpcb.7b01427</a>

Alternative languages

  • Result language

    angličtina

  • Original language name

    Side Reactions with an Equilibrium Constraint: Detailed Mechanism of the Substitution Reaction of Tetraplatin with dGMP as a Starting Step of the Platinum(IV) Reduction Process

  • Original language description

    Two possible pathways of the substitution reaction within the reduction process of the Pt-IV(DACH)Cl-4 by dGMP are compared: associative reaction course and autocatalytic Basolo-Pearson mechanisms. Since two forms: single-protonated and fully deprotonated phosphate group of dGMP are present in equilibrium at neutral and mildly acidic solutions, consideration of a side reactions scheme with acido-basic equilibrium-constraint is a very important model for obtaining reliable results. The examined complexes are optimized at the B3LYP-GD3BJ/6-31G(d)level with the COSMO implicit solvation model and Klamt&apos;s radii used for cavity construction. Energy characteristics and thermodynamics for all reaction branches are determined using the B3LYP-GD3BJ/6-311++G(2df,2pd)/IEF-PCM/scaled-UAKS level with Wertz&apos;s entropy corrections. Rate constants are estimated for each individual branch according to Eyring&apos;s transition state theory (TST), averaged according to equilibrium constraint and compared with available experimental data. The determined reaction barriers of the autocatalytic pathway fairly correspond with experimental values. Furthermore, autocatalytic reaction of tetraplatin and its two analogues complexes [Pt-IV(en)Cl-4 and Pt-IV(NH3)(2)Cl-4] are explored and compared with measured data in order to examined general reaction descriptors.

  • Czech name

  • Czech description

Classification

  • Type

    J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database

  • CEP classification

  • OECD FORD branch

    10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Result continuities

  • Project

    <a href="/en/project/GA16-06240S" target="_blank" >GA16-06240S: Structure and dynamics of organometallic complexes in bio-environment.</a><br>

  • Continuities

    P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Others

  • Publication year

    2017

  • Confidentiality

    S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Data specific for result type

  • Name of the periodical

    Journal of Physical Chemistry B

  • ISSN

    1520-6106

  • e-ISSN

  • Volume of the periodical

    121

  • Issue of the periodical within the volume

    17

  • Country of publishing house

    US - UNITED STATES

  • Number of pages

    14

  • Pages from-to

    4400-4413

  • UT code for WoS article

    000400881300008

  • EID of the result in the Scopus database