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Unravelling the Biosynthetic Flexibility of UK-2A Enables Enzymatic Synthesis of Its Structural Variants

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논문

Unravelling the Biosynthetic Flexibility of UK-2A Enables Enzymatic Synthesis of Its Structural Variants

학술지

ACS Synthetic biology

저자명

Tan, Hongqun; Yang, Xuejun; Dai, Qi; Deng, Zixin; Qu, Xudong

초록

<P>Emerging antimicrobial resistant fungal pathogens are a growing threat, and fungicides with novel modes of action are urgently needed to prevent critical failures in global food security. Fenpicoxamid, the prodrug of UK-2A, is a member of a new class of antifungal agents that displays no cross-resistance to other fungicides. Rational engineering of its structure using a biosynthetic approach is a promising avenue for developing more potent fungicides. Herein, through <I>in vitro</I> enzymatic reconstitution, we elucidate the biosynthetic pathway of UK-2A. Its biosynthesis involves a flexible AMP-binding protein and dilactone formation assembly enzymes that are able to select and incorporate highly diverse substituted salicylic acids into the dilactone scaffold. By introducing diverse salicylic acids into the <I>in vitro</I> biosynthetic pathway, we successfully generate 14 novel deacyl UK-2A analogues. This study reveals the flexibility of the biosynthetic pathway of UK-2A and provides an effective solution to rationally engineer its crucial C3 moiety.</P><BR>[FIG OMISSION]</BR>

발행연도

2019

발행기관

American Chemical Society

ISSN

2161-5063

8

12

페이지

pp.2659-2665

주제어

biosynthesis; rational engineering; enzymatic synthesis; polyketide; fungicide; dilactone

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2 2023-12-11

논문; 2019-12-31

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