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Entropy-based rational modulation of the pKa of a synthetic pH-dependent nanoswitch.

著者 Mariottini D , Idili A , Nijenhuis MAD , Ercolani G , Ricci F
J Am Chem Soc.2019 Jul 11 ; ():.
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The rational regulation of the pKa of an ionisable 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 to loop formation and is gradually shifted to more basic pH values when the length of the linker domain is reduced. Through mathematical modelling 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.
PMID: 31296004 [PubMed - as supplied by publisher]
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