Promoting the glycosylation of drug-like natural products in a Saccharomyces cerevisiae chassis by deletion of endogenous glycosidases
文献类型： 外文期刊
作者： Huang, Yingying 1 ; Zhong, Weimao 1 ; Varga, Kinga E. 5 ; Benko, Zsigmond 5 ; Pocsi, Istvan 1 ; Yang, Chenglong 2 ; Molnar, Istvan 6 ;
作者机构： 1.Univ Arizona, Southwest Ctr Nat Prod Res, Tucson, AZ USA
2.Fujian Acad Agr Sci, Inst Food Sci & Technol, Fuzhou, Peoples R China
3.Minist Agr & Rural Affairs, Coconstruct Minist & Prov, Key Lab Subtrop Characterist Fruits Vegetables & E, Fuzhou, Peoples R China
4.Fujian Key Lab Agr Prod Food Proc, Fuzhou, Peoples R China
5.Univ Debrecen, Inst Biotechnol, Fac Sci & Technol, Dept Mol Biotechnol & Microbiol, H-4032 Debrecen, Hungary
6.VTT Tech Res Ctr Finland, Espoo, Finland
7.Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
关键词： Glycodiversification; Combinatorial biosynthesis; Biocatalysis; Polyketide; Flavonoid; Stilbene; Exoglycanase
期刊名称：BIORESOURCE TECHNOLOGY （ 影响因子：9.0； 五年影响因子：9.5 ）
ISSN： 0960-8524
年卷期： 2025 年 422 卷
页码：
收录情况： SCI
摘要： Glycosylation is an effective strategy to improve the absorption, distribution, metabolism, excretion, and toxicity of natural product (NP) pharmacophores. While heterologous production of broad-spectrum fungal glucosyltransferases such as BbGT86 of Beauveria bassiana yields varied phenolic glucoconjugates in S. cerevisiae, endogenous yeast glycosidases diminish the conversion yields and limit the structural diversity of the products. We set out to improve the efficiency and broaden the regiospecificity of the glucosylation of NPs or their unnatural product analogues (uNPs). Using yeast strains deficient in exoglycanases EXG1 or SPR1, we evaluated total biosynthetic and biocatalytic synthetic biology platforms to produce glycoconjugates from polyketides of the benzenediol lactone family, and polyphenols of the phenylpropanoid class. We show that for 13 out of the 18 aglycons tested, exoglycanase deletions improve glucoside yields and/or alter glucoconjugate regioisomer distributions, while macrolactone glycoconjugates with an aryl methylene ketone moiety are impervious to hydrolysis by EXG1. We demonstrate that elimination of EXG1 or biosynthetic methylation of glucosides are efficient alternative strategies to differentially modulate glycoside regioisomer profiles for future pharmaceutical, nutraceutical or crop protection applications.
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