Glycyl Radical Enzymes Catalyzing the Dehydration of Two Isomers of N-Methyl-4-hydroxyproline

doi:10.1021/acscatal.4c00216

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	Glycyl Radical Enzymes Catalyzing the Dehydration of Two Isomers of N-Methyl-4-hydroxyproline
	Jiang, Li 1,2,3,4,5; Yang, Yiqian 6; Huang, Lin 2; Zhou, Yan 2; An, Junwei 2; Zheng, Yuchun 1; Chen, Yiwei 1; Liu, Yanhong 7; Huang, Jianhui 2; Ang, Ee Lui 8; Zhao, Suwen9,10 ; Zhao, Huimin 11; Liao, Rongzhen 6; Wei, Yifeng 8; Zhang, Yan 1,2,3,4,5
	2024
发表期刊	ACS CATALYSIS (IF:11.3[JCR-2023],12.6[5-Year])
ISSN	2155-5435
EISSN	2155-5435
卷号	14 期号:7 页码:4407-4422
发表状态	已发表
DOI	10.1021/acscatal.4c00216
摘要	The various isomers of hydroxyproline (HP) are widely distributed in nature, serving as key components of structural proteins, while their quaternized betaine derivatives function as osmoprotectants in many organisms. Aerobic bacteria degrade HPs through a variety of well-studied mechanisms. Recent studies show that certain anaerobic bacteria degrade HPs through distinct mechanisms, involving the O2-sensitive glycyl radical enzymes (GREs) t4L-HP dehydratase (HypD) and t4D-HP C-N lyase (HplG). Here, we report the discovery of two more GREs, N-methyl c4L-HP dehydratase (HpyG) and N-methyl c4D-HP dehydratase (HpzG), which catalyze radical-mediated dehydration of the two N-methyl-c4HP enantiomers, while also displaying significant activities toward their unmethylated substrates. Both GREs are associated with homologues of pyrroline-5-carboxylate reductase, which catalyze reduction of their products N-methyl-pyrroline-5-carboxylate to form N-methyl-proline. Crystal structures of HpyG and HpzG in complex with their substrates revealed active site architectures distinct from that of HypD and provided insights into the mechanism of enantioselective radical-mediated dehydration. Our research further expands the repertoire of diverse chemical mechanisms involved in the bacterial metabolism of highly prevalent HP isomers and derivatives in the anaerobic biosphere. © 2024 American Chemical Society.
关键词	Biodegradation Collagen Crystal structure Dehydration Enantiomers Enzymes Hydroxyproline 4 hydroxyprolines 4-hydroxyproline Catalyse Crystals structures Glycyl radical enzyme N-methyl-hydroxyproline Pyrrolines QM calculation Radical enzymes Structural proteins
收录类别	EI
语种	英语
出版者	American Chemical Society
EI入藏号	20241115737406
EI主题词	Enantioselectivity
EI分类号	461 Bioengineering and Biology ; 461.8 Biotechnology ; 801.2 Biochemistry ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 804.1 Organic Compounds ; 933.1.1 Crystal Lattice
原始文献类型	Article in Press
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/352554
专题	iHuman研究所生命科学与技术学院 iHuman研究所_PI研究组_赵素文组
通讯作者	Liao, Rongzhen; Wei, Yifeng; Zhang, Yan
作者单位	1.New Cornerstone Science Laboratory, School of Pharmaceutical Science and Technology, Tianjin University, Tianjin; 300072, China; 2.Tianjin Key Laboratory for Modern Drug Delivery & High-Efficiency, Collaborative Innovation Center of Chemical Science and Engineering, School of Pharmaceutical Science and Technology, Tianjin University, Tianjin; 300072, China; 3.Frontiers Science Center for Synthetic Biology (Ministry of Education), Tianjin University, Tianjin; 300072, China; 4.Key Laboratory of Systems Bioengineering (Ministry of Education), School of Chemical Engineering and Technology, Tianjin University, Tianjin; 300072, China; 5.Department of Chemistry, Tianjin University, Tianjin; 300072, China; 6.Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, Hubei Key Laboratory of Materials Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan; 430074, China; 7.Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing; 100190, China; 8.Singapore Institute of Food and Biotechnology Innovation, Agency for Science, Technology and Research (A*STAR), Singapore; 138669, Singapore; 9.iHuman Institute, ShanghaiTech University, Shanghai; 201210, China; 10.School of Life Science and Technology, ShanghaiTech University, Shanghai; 201210, China; 11.Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana─Champaign, 600 South Mathews Avenue, Urbana; IL; 61801, United States
推荐引用方式 GB/T 7714	Jiang, Li,Yang, Yiqian,Huang, Lin,et al. Glycyl Radical Enzymes Catalyzing the Dehydration of Two Isomers of N-Methyl-4-hydroxyproline[J]. ACS CATALYSIS,2024,14(7):4407-4422.
APA	Jiang, Li.,Yang, Yiqian.,Huang, Lin.,Zhou, Yan.,An, Junwei.,...&Zhang, Yan.(2024).Glycyl Radical Enzymes Catalyzing the Dehydration of Two Isomers of N-Methyl-4-hydroxyproline.ACS CATALYSIS,14(7),4407-4422.
MLA	Jiang, Li,et al."Glycyl Radical Enzymes Catalyzing the Dehydration of Two Isomers of N-Methyl-4-hydroxyproline".ACS CATALYSIS 14.7(2024):4407-4422.