title: Evident and latent plasticity across the rice diterpene synthase family with potential implications for the evolution of diterpenoid metabolism in the cereals.
abstract: The evolution of natural product biosynthetic pathways can be envisioned to occur via a number of mechanisms. In the present study we provide evidence that latent plasticity plays a role in such metabolic evolution. In particular, rice (Oryza sativa) produces both ent- and syn-CPP (copalyl diphosphate), which are substrates for downstream diterpene synthases. In the present paper we report that several members of this enzymatic family exhibit dual reactivity with some pairing of ent-, syn- or normal CPP stereochemistry. Evident plasticity was observed, as a previously reported ent-sandaracopimaradiene synthase also converts syn-CPP into syn-labda-8(17),12E,14-triene, which can be found in planta. Notably, normal CPP is not naturally found in rice. Thus the presence of diterpene synthases that react with this non-native metabolite reveals latent enzymatic/metabolic plasticity, providing biochemical capacity for utilization of such a novel substrate (i.e. normal CPP) which may arise during evolution, the implications of which are discussed.
authors.affiliation: Department of Biochemistry, Biophysics and Molecular Biology, Iowa State University, Ames, IA 50011, USA.
authors.forename: Dana
authors.initials: D
authors.lastname: Morrone
authors.forename: Matthew L
authors.initials: ML
authors.lastname: Hillwig
authors.forename: Matthew E
authors.initials: ME
authors.lastname: Mead
authors.forename: Luke
authors.initials: L
authors.lastname: Lowry
authors.forename: D Bruce
authors.initials: DB
authors.lastname: Fulton
authors.forename: Reuben J
authors.initials: RJ
authors.lastname: Peters
mesh_terms: D019883:Alkyl and Aryl Transferases / Q000145:classification / Q000235:genetics / Q000378:metabolism*; D005075:Biological Evolution; D004224:Diterpenes / Q000378:metabolism*; D015971:Gene Expression Regulation, Enzymologic; D018506:Gene Expression Regulation, Plant / Q000502:physiology*; D015394:Molecular Structure; D010755:Organophosphates / Q000737:chemistry / Q000378:metabolism; D012275:Oryza / Q000201:enzymology* / Q000235:genetics; D018515:Plant Leaves / Q000201:enzymology; D010940:Plant Proteins / Q000235:genetics / Q000378:metabolism*; D013237:Stereoisomerism; D013379:Substrate Specificity
chemical_list: D004224:Diterpenes; D010755:Organophosphates; D010940:Plant Proteins; C408747:copalyl diphosphate; D019883:Alkyl and Aryl Transferases; C108877:terpene synthase