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化学蛋白质组学分析揭示绿原酸是脱氢抗坏血酸还原酶1的共价抑制剂。

Chemoproteomic Profiling Reveals Chlorogenic Acid as a Covalent Inhibitor of Dehydroascorbate Reductase 1.

作者信息

Xu Jingyuan, Chen Lijun, Wang Shanshan, Zhang Wen, Liang Jianjia, Ran Lu, Deng Zhangshuang, Zhou Yiqing

机构信息

School of Biotechnology and Food Engineering, Changshu Institute of Technology, Suzhou 215500, China.

Hubei Key Laboratory of Natural Products Research and Development, College of Biological and Pharmaceutical Sciences, China Three Gorges University, Yichang 443002, China.

出版信息

J Agric Food Chem. 2025 Jan 8;73(1):908-918. doi: 10.1021/acs.jafc.4c07955. Epub 2024 Dec 20.

DOI:10.1021/acs.jafc.4c07955
PMID:39704675
Abstract

Chlorogenic acid (CA) is an abundant plant secondary metabolite with promising allelopathic effects on weed growth. However, the molecular targets and mechanism of action of CA in plants remain elusive. Here, we report the employment of a clickable photoaffinity probe in identifying the protein targets of CA in seedling proteomes. CA specifically binds dehydroascorbate reductase 1 (DHAR1), an enzyme responsible for ascorbate regeneration in plants, by covalent alkylating Cys20 within the catalytic center, thereby inhibiting its activity. In vivo application of CA reduced the pool size and redox state of ascorbate, leading to HO accumulation in seedlings. In agreement with these results, CA significantly induced the upregulation of antioxidant enzymes and downregulation of proteins involved in water transport and photosynthesis, as evidenced by quantitative proteomics. Taken together, this study revealed DHAR1 as a functional target underlying CA's allelopathic activity in plants, which opens new opportunities for the development of novel herbicides from naturally existing resources.

摘要

绿原酸(CA)是一种丰富的植物次生代谢产物,对杂草生长具有潜在的化感作用。然而,CA在植物中的分子靶点和作用机制仍不清楚。在此,我们报告了使用一种可点击的光亲和探针来鉴定幼苗蛋白质组中CA的蛋白质靶点。CA通过共价烷基化催化中心内的Cys20,特异性结合脱氢抗坏血酸还原酶1(DHAR1),该酶负责植物中抗坏血酸的再生,从而抑制其活性。CA的体内应用减少了抗坏血酸的库大小和氧化还原状态,导致幼苗中HO积累。与这些结果一致,定量蛋白质组学表明,CA显著诱导了抗氧化酶的上调以及参与水分运输和光合作用的蛋白质的下调。综上所述,本研究揭示了DHAR1是CA在植物中化感活性的功能靶点,这为从天然资源开发新型除草剂开辟了新机会。

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