Oja Terhi, Palmu Kaisa, Lehmussola Hanna, Leppäranta Outi, Hännikäinen Kati, Niemi Jarmo, Mäntsälä Pekka, Metsä-Ketelä Mikko
Department of Biochemistry and Food Chemistry, University of Turku, FIN-20014 Turku, Finland.
Chem Biol. 2008 Oct 20;15(10):1046-57. doi: 10.1016/j.chembiol.2008.07.022.
Alnumycin is closely related to the benzoisochromanequinone (BIQ) polyketides such as actinorhodin. Exceptional structural features include differences in aglycone tailoring that result in the unique alnumycin chromophore and the existence of an unusual 4-hydroxymethyl-5-hydroxy-1,3-dioxan moiety. Cloning and sequencing of the alnumycin gene cluster from Streptomyces sp. CM020 revealed expected biosynthesis genes for polyketide assembly, but several genes encoding subsequent tailoring enzymes were highly atypical. Heterologous expression studies confirmed that all of the genes required for alnumycin biosynthesis resided within the sequenced clone. Inactivation of genes aln4 and aln5 showed that the mechanism of pyran ring formation differs from actinorhodin and granaticin pathways. Further inactivation studies identified two genes, alnA and alnB, involved in the synthesis and attachment of the dioxan moiety, and resulted in the production of the polyketide prealnumycin.
阿努霉素与诸如放线紫红素等苯并异色满醌(BIQ)聚酮化合物密切相关。其独特的结构特征包括糖苷配基修饰的差异,这导致了阿努霉素独特的发色团,以及存在一个不寻常的4-羟甲基-5-羟基-1,3-二氧六环部分。来自链霉菌属CM020的阿努霉素基因簇的克隆和测序揭示了聚酮化合物组装的预期生物合成基因,但几个编码后续修饰酶的基因非常不典型。异源表达研究证实,阿努霉素生物合成所需的所有基因都存在于测序克隆中。aln4和aln5基因的失活表明,吡喃环形成机制与放线紫红素和石榴菌素途径不同。进一步的失活研究确定了两个与二氧六环部分的合成和连接有关的基因alnA和alnB,并导致了聚酮化合物前阿努霉素的产生。