Although one of an enzyme's hallmarks is the high specificity for their natural substrates, substrate promiscuity has been reported more frequently. It is known that promiscuous enzymes generally show different catalytic efficiencies to different substrates, but our understanding of the origin of such differences is still lacking. Here we report the results of quantum mechanical/molecular mechanical simulations and an experimental study of salicylic acid binding protein 2 (SABP2). SABP2 has promiscuous esterase activity toward a series of substrates but shows a high activity toward its natural substrate, methyl salicylate (MeSA). Our results demonstrate that this enzyme may use substrate-assisted catalysis involving the hydroxyl group from MeSA to enhance the activity and achieve substrate discrimination.
Gibberellins (GAs) are a major class of plant hormones that regulates diverse developmental programs. Both acquiring abilities to synthesize GAs and evolving divergent GA receptors have been demonstrated to play critical roles in the evolution of land plants. In contrast, little is understood regarding the role of GA‐inactivating mechanisms in plant evolution. Here we report on the origin and evolution of GA methyltransferases (GAMTs), enzymes that deactivate GAs by converting bioactive GAs to inactive GA methylesters. Prior to this study,
GAMT
genes, which belong to the SABATH family, were known only from
Arabidopsis
. Through systematic searches for
SABATH
genes in the genomes of 260 sequenced land plants and phylogenetic analyses, we have identified a putative
GAMT
clade specific to seed plants. We have further demonstrated that both gymnosperm and angiosperm representatives of this clade encode active methyltransferases for GA methylation, indicating that they are functional orthologs of
GAMT
. In seven selected seed plants,
GAMT
genes were mainly expressed in flowers and/or seeds, indicating a conserved biological role in reproduction.
GAMT
genes are represented by a single copy in most species, if present, but multiple copies mainly produced by whole genome duplications have been retained in Brassicaceae. Surprisingly, more than 2/3 of the 248 flowering plants examined here lack
GAMT
genes, including all species of Poales (e.g., grasses), Fabales (legumes), and the large Superasterid clade of eudicots. With these observations, we discuss the significance of
GAMT
origination, functional conservation and diversification, and frequent loss during the evolution of flowering plants.
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