Nucleotide aggregation in aqueous solution. A multicomponent self-diffusion study |
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Authors: | R Rymdén P Stilbs |
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Institution: | Institute of Physical Chemistry, Uppsala University, Box 532, S - 751 21 Uppsala, Sweden |
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Abstract: | The self-aggregation of the mononucleotides (AMP, CMP, GMP and UMP) and caffeine up to their solubility limit in 2H2O has been monitored through self-diffusion measurements, using the Fourier transform NMR pulsed-gradient spin-echo self-diffusion technique. The data were iteratively fitted to a number of aggregation models. It was concluded that the best agreement between simulations and experiment for the mononucleotides was obtained for a 'semi-isodesmic', indefinite aggregation model (also known as a Type III SEK or cooperative indefinite self-association model), where the first (dimerization) aggregation constant is a magnitude lower than those for the higher aggregation steps. Typical values were 0.4 and 6 l mol-1, respectively. Under these conditions, the main fraction of solute is monomeric throughout the concentration range and the distribution of higher oligomers is very broad. Caffeine self-aggregation is clearly different and is consistent with several aggregation models. The mixed aggregation of caffeine (at a low total concentration) and the mononucleotides was successfully monitored in an extension of the basic study. It was found that caffeine binding to mononucleotide aggregates increases in the series UMP, CMP, GMP and AMP. |
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Keywords: | Self- diffusion Stacking Aggregation Nucleolide NMR |
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