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Genetically Encoded Benzoyllysines Serve as Versatile Probes for Interrogating Histone Benzoylation and Interactions in Living Cells

文献类型：期刊论文

作者Tian, Hongtao2,3; Yang, Jiale2,3; Guo, An-Di2,3; Ran, Yu4; Yang, Yun-Zhi2; Yang, Bing4; Huang, Ruimin2,3; Liu, Haiming1; Chen, Xiao-Hua2,3,5
刊名ACS CHEMICAL BIOLOGY
出版日期2021-11-19
卷号16期号:11页码:2560-2569
ISSN号1554-8929
DOI10.1021/acschembio.1c00614
通讯作者Liu, Haiming(liuhm@shanghaitech.edu.cn) ; Chen, Xiao-Hua(xhchen@simm.ac.cn)
英文摘要Histone posttranslational modifications (PTMs) are vital epigenetic regulators in many fundamental cell signaling pathways and diverse biological processes. Histone lysine benzoylation is a recently identified epigenetic mark associated with active transcription; however, it remains to be explored. Herein, we first report the genetic encoding of benzoyllysine and fluorinated benzoyllysines into full-length histone proteins in a site-specific manner in live cells, based on our rationally designed synthetase and fine-integrated fluorine element into benzoyllysines. The incorporated unnatural amino acids integrating unique features were demonstrated as versatile probes for investigating histone benzoylation under biological environments, conferring multiplex signals such as F-19 NMR spectra with chemical clarity and fluorescence signals for benzoylation. Moreover, the site specifically incorporated lysine benzoylation within native full-length histone proteins revealed distinct dynamics of debenzoylation in the presence of debenzoylase sirtuin 2 (SIRT2). Our developed strategy for genetic encoding of benzoyllysines offers a general and novel approach to gain insights into interactions of site-specific histone benzoylation modifications with interactomes and molecular mechanisms in physiological settings, which could not be accessible with fragment histone peptides. This versatile chemical tool enables a direct and new avenue to explore benzoylation, interactions, and histone epigenetics, which will provide broad utilities in chemical biology, protein science, and basic biology research.
WOS关键词TRANSFER-RNA SYNTHETASE ; F-19 NMR ; METABOLIC-REGULATION ; GENE-EXPRESSION ; SODIUM BENZOATE ; AMINO-ACIDS ; LYSINE ; CODE ; PROTEINS ; IDENTIFICATION
资助项目National Science Foundation of China (NSFC)[21778062] ; National Science Foundation of China (NSFC)[92053106] ; Science and Technology Commission of Shanghai Municipality, China[18431907100] ; ShanghaiTech University ; Analytical Instrumentation Center at ShanghaiTech University[SPSTAIC10112914]
WOS研究方向Biochemistry & Molecular Biology
语种英语
WOS记录号WOS:000771488700004
出版者AMER CHEMICAL SOC
源URL[http://119.78.100.183/handle/2S10ELR8/300024]  
专题中国科学院上海药物研究所
通讯作者Liu, Haiming; Chen, Xiao-Hua
作者单位1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Mat Med, Shanghai 201203, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Zhejiang Univ, Life Sci Inst, Hangzhou 310058, Peoples R China
5.Univ Chinese Acad Sci, Sch Pharmaceut Sci & Technol, Hangzhou Inst Adv Study, Hangzhou 310024, Peoples R China
推荐引用方式
GB/T 7714		 Tian, Hongtao,Yang, Jiale,Guo, An-Di,et al. Genetically Encoded Benzoyllysines Serve as Versatile Probes for Interrogating Histone Benzoylation and Interactions in Living Cells[J]. ACS CHEMICAL BIOLOGY,2021,16(11):2560-2569.
APA Tian, Hongtao.,Yang, Jiale.,Guo, An-Di.,Ran, Yu.,Yang, Yun-Zhi.,...&Chen, Xiao-Hua.(2021).Genetically Encoded Benzoyllysines Serve as Versatile Probes for Interrogating Histone Benzoylation and Interactions in Living Cells.ACS CHEMICAL BIOLOGY,16(11),2560-2569.
MLA Tian, Hongtao,et al."Genetically Encoded Benzoyllysines Serve as Versatile Probes for Interrogating Histone Benzoylation and Interactions in Living Cells".ACS CHEMICAL BIOLOGY 16.11(2021):2560-2569.

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来源：上海药物研究所

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