Corrin Ring Modifications Reveal the Chemical and Spatial Requirements for the B12btuB Riboswitch Interaction

Author:

Musiari Anastasia1,Reichenbach María1ORCID,Gallo Sofia1,Sigel Roland K. O.1ORCID

Affiliation:

1. Department of Chemistry University of Zurich Winterthurerstrasse 190 CH-8057 Zurich Switzerland

Abstract

AbstractThe btuB riboswitch is a regulatory RNA sequence controlling gene expression of the outer membrane B12 transport protein BtuB by specifically binding coenzyme B12 (AdoCbl) as its natural ligand. The B12 sensing riboswitch class is known to accept various B12 derivatives, leading to a division into two riboswitch subclasses, dependent on the size of the apical ligand. Here we focus on the role of side chains b and e on affinity and proper recognition, i. e. correct structural switch of the btuB RNA, which belongs to the AdoCbl‐binding class I. Chemical modification of these side chains disturbs crucial hydrogen bonds and/or electrostatic interactions with the RNA, its effect on both affinity and switching being monitored by in‐line probing. Chemical modifications at sidechain b of vitamin B12 show larger effects indicating crucial B12‐RNA interactions. When introducing the same modification to AdoCbl the influence of any side‐chain modification tested is reduced. This renders the impact of the adenosyl‐ligand for B12btuB riboswitch recognition clearly beyond the known role in affinity.

Funder

Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung

European Research Council

Universität Zürich

Publisher

Wiley

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