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Entropy-Based Rational Modulation of the pKa of a Synthetic pH-Dependent Nanoswitch.
Mariottini, Davide; Idili, Andrea; Nijenhuis, Minke A D; Ercolani, Gianfranco; Ricci, Francesco.
Afiliación
  • Mariottini D; Chemistry Department , University of Rome, Tor Vergata , Via della Ricerca Scientifica , 00133 Rome , Italy.
  • Idili A; Chemistry Department , University of Rome, Tor Vergata , Via della Ricerca Scientifica , 00133 Rome , Italy.
  • Nijenhuis MAD; Interdisciplinary Nanoscience Center (iNANO), Aarhus University , DK-8000 Aarhus C , Denmark.
  • Ercolani G; Chemistry Department , University of Rome, Tor Vergata , Via della Ricerca Scientifica , 00133 Rome , Italy.
  • Ricci F; Chemistry Department , University of Rome, Tor Vergata , Via della Ricerca Scientifica , 00133 Rome , Italy.
J Am Chem Soc ; 141(29): 11367-11371, 2019 07 24.
Article en En | MEDLINE | ID: mdl-31296004
The rational regulation of the pKa of an ionizable group in a synthetic device could be achieved by controlling the entropy of the linker connecting the hydrogen bond forming domains. We demonstrate this by designing a set of pH-responsive synthetic DNA-based nanoswitches that share the same hydrogen bond forming domains but differ in the length of the linker. The observed acidic constant (pKa) of these pH-dependent nanoswitches is linearly dependent on the entropic cost associated with loop formation and is gradually shifted to more basic pH values when the length of the linker domain is reduced. Through mathematical modeling and thermodynamic characterization we demonstrate that the modulation of the observed pKa is due to a purely entropic contribution. This approach represents a very versatile strategy to rationally modulate the pKa of synthetic devices in a highly predictable and accurate way.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Tipo de estudio: Prognostic_studies Idioma: En Revista: J Am Chem Soc Año: 2019 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Estados Unidos
Texto completo
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Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Tipo de estudio: Prognostic_studies Idioma: En Revista: J Am Chem Soc Año: 2019 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Estados Unidos