The RNA strand in an RNA/DNA duplex with unpaired
ribonucleotides can undergo self-cleavage at bulge sites
in the presence of a variety of divalent metal ions (Hüsken
et al., Biochemistry, 1996, 35:16591–16600).
Transesterification proceeds via an in-line mechanism,
with the 2′-OH of the bulged nucleotide attacking
the 3′-adjacent phosphate group. The site-specificity
of the reaction is most likely a consequence of the greater
local conformational freedom of the RNA backbone in the
bulge region. A standard A-form backbone geometry prohibits
formation of an in-line arrangement between 2′-oxygen
and phosphate. However, the backbone in the region of an
unpaired nucleotide appears to be conducive to an in-line
approach. Therefore, the bulge-mediated phosphoryl transfer
reaction represents one of the simplest RNA self-cleavage
systems. Here we focus on the conformational features of
the RNA that underlie site-specific cleavage. The structures
of an RNA/DNA duplex with single ribo-adenosyl bulges were
analyzed in two crystal forms, permitting observation of
10 individual conformations of the RNA bulge moiety. The
bulge geometries cover a range of relative arrangements
between the 2′-oxygen of the bulged nucleotide and
the P-O5′ bond (including adjacent and near
in-line) and give a detailed picture of the conformational
changes necessary to line up the 2′-OH nucleophile
and scissile bond. Although metal ions are of crucial importance
in the catalysis of analogous cleavage reactions by ribozymes,
it is clear that local strain or conformational flexibility
in the RNA also affect cleavage selectivity and rate (Soukup
& Breaker, RNA, 1999, 5:1308–1325).
The geometries of the RNA bulges frozen out in the crystals
provide snapshots along the reaction pathway prior to the
transition state of the phosphoryl transfer reaction.