Nucleotide coordination with 14 lanthanides studied by isothermal titration calorimetry
Loading...
Date
2017-06-09
Authors
Zhang, Zijie
Morishita, Kiyoshi
Lin, Wei Ting David
Huang, Po-Jung Jimmy
Liu, Juewen
Journal Title
Journal ISSN
Volume Title
Publisher
Elsevier
Abstract
With their hydrolytic, optical and magnetic properties, lanthanide ions (Ln3+) are versatile probes for nucleic acids. In addition, nucleotide-coordinated Ln3+ ions form useful nanoparticles. However, the thermodynamic basis of their interaction is still lacking. In this work, isothermal titration calorimetry (ITC) is used to study the binding between nucleotides and 14 different Ln3+ ions. Ln3+ interacts mainly with the phosphate of cytidine and thymidine monophosphate (CMP and TMP), while the nucleobases in adenosine and guanosine monophosphate (AMP and GMP) are also involved. Phosphate binding is fully entropy driven since the reactions absorb heat. Nucleosides alone do not bind Ln3+ and the purines need the phosphate for chelation. With increasing atomic number of Ln3+, the binding reaction with GMP goes from exothermic to endothermic. The entropy contribution starts to increase from Gd3+, explaining the ‘gadolinium break’ observed in many Ln3+-mediated RNA cleavage reactions. This study provides fundamental insights into the Ln3+/nucleotide interactions, and it is useful for understanding related biosensors, nanomaterials, catalysts, and for lanthanide separation.
Description
The final publication is available at Elsevier via http://dx.doi.org/10.1016/j.cclet.2017.06.014 © 2017. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/
Keywords
DNA, Entropy, Lanthanides, Metal ions, Nucleic acids