Effects of hydration on the acid-base interactions and secondary structures of poly-L-lysine probed by 15N and 13C solid state NMR

Physical Chemistry Chemical Physics : PCCP
Alexandra DosHans-Heinrich Limbach

Abstract

Using high resolution solid state (15)N and (13)C NMR spectroscopy we have studied the effects of successive hydration on the (15)N labeled side chain amino groups of solid poly-L-lysine (PLL) in the presence of acids. Generally, hydration leads to the formation of local "ionic fluid" phases composed by flexible side chain ammonium groups, acid anions and small amounts of water. The associated local dynamics reduces the widths of the inhomogeneously broadened (15)N amino signals found for the dry states. The hydration of free base PLL--which consists of mixtures of alpha-helices and beta-pleated sheets--is monitored by a small low-field shift of the amino group signal arising from hydrogen bonding with water, reaching eventually the value of PLL in water at pH 13. No difference for the two conformations is observed. PLL x HF adopts a similar secondary structure with isolated NHF hydrogen bonds; hydration leads only to small low-field shifts which are nevertheless compatible with the formation of ammonium groups in aqueous solution. PLL doped with small amounts of HCl contains ammonium groups which are internally solvated by neighboring free amino groups. Both nitrogen environments are characterized by different chemical shifts....Continue Reading

References

Feb 1, 1977·Biopolymers·M Suwalsky, A Llanos
Sep 1, 1973·Archives of Biochemistry and Biophysics·H Saitô, I C Smith
May 1, 1965·Journal of Molecular Biology·U SHMUELI, W TRAUB
Aug 22, 2006·Biophysical Chemistry·M Rozenberg, G Shoham
Mar 21, 2007·Journal of the American Chemical Society·Shasad SharifHans-Heinrich Limbach
Mar 29, 2007·The Journal of Physical Chemistry. B·Shasad SharifHans-Heinrich Limbach
Apr 26, 2007·Journal of the American Chemical Society·Shasad SharifHans-Heinrich Limbach
Jul 14, 2007·Journal of the American Chemical Society·Shasad SharifHans-Heinrich Limbach

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