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Activated ribonucleotides undergo a sugar pucker switch upon binding to a single-stranded RNA template
Na Zhang1, Shenglong Zhang, Jack W Szostak
1Howard Hughes Medical Institute and Department of Molecular Biology and Center for Computational and Integrative Biology, Massachusetts General Hospital, 185 Cambridge Street, Boston, Massachusetts 02114, USA.
Journal of the American Chemical Society
|February 3, 2012
Summary
Activated ribonucleotides switch sugar conformation upon binding to RNA templates, enhancing nonenzymatic RNA replication. This conformational change explains why RNA monomers and templates are superior for origin-of-life polymerization models.
Area of Science:
- Origin of Life Studies
- Biochemistry
- Molecular Evolution
Background:
- Nonenzymatic RNA replication is a key model for early life.
- Efficient RNA copying requires specific monomer and template conformations (A-form, C3'-endo).
- Free ribonucleotides typically adopt a C2'-endo sugar pucker, hindering polymerization.
Purpose of the Study:
- To investigate the conformational changes of ribonucleotides upon binding to oligonucleotide templates.
- To determine if a sugar pucker switch occurs and its role in template-directed polymerization.
- To compare RNA vs. DNA template interactions with activated nucleotides.
Main Methods:
- Utilized transferred nuclear Overhauser effect spectroscopy (TrNOESY).
- Analyzed interactions between nucleotide 5'-phosphorimidazolides and single-stranded oligonucleotide templates.
- Studied both activated ribonucleotides and deoxyribonucleotides on RNA and DNA templates.
Main Results:
- Activated ribonucleotides switch from C2'-endo to C3'-endo sugar pucker upon binding to RNA templates.
- This conformational switch is specific to RNA templates; it does not occur on DNA templates.
- Activated 2'-deoxyribonucleotides maintain a C2'-endo conformation regardless of template type.
Conclusions:
- A sugar pucker conformational switch upon template binding enhances ribonucleotide polymerization.
- This finding provides a structural basis for the superior efficiency of RNA over DNA in nonenzymatic replication.
- Supports the role of RNA in the origin of life and early genetic systems.
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