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Discovery, Mechanism, and Bioproduction Studies of a Moss-Derived Microbial-like Terpene Synthase CrMTPSL3 Generating the Tricyclic Sphaeroane Scaffold

文献类型：期刊论文

作者Li, Xin1,4; Liu, Yuanning3; Chen, Jiaxing1,2; Wang, Chen3; Chen, Bao1,4; Liu, Lijun1; Liu, Xuemeng1; Chen, Xiaochen1; Zhao, Yao1; He, Ting1
刊名ACS CATALYSIS
出版日期2025-11-18
页码8
关键词Terpene synthase Sphaeroane Mechanism Deuterium-scanning Bioproduction
ISSN号2155-5435
DOI10.1021/acscatal.5c06284
通讯作者Xu, Zhengren(zhengrenxu@bjmu.edu.cn) ; Xu, Baofu(bfxu@simm.ac.cn)
英文摘要The sphaeroane diterpenoids are natural products with a tricyclic scaffold, yet the biosynthetic mechanism remains unclear. We characterized a sphaeroane diterpene synthase, CrMTPSL3, from Claopodium rostratum. Chemical computation together with crystallization experiments determined the absolute stereochemistry of the products. Further deuterium-scanning experiments supported CrMTPSL3 forms the sphaeroane scaffold sequentially as GGPP isomerization, 1,11- and 10,14-cyclizations, two successive 1,2-hydride shifts, 1,2-methyl shift, 1,2-hydride transfer of the pro-S hydrogen, 1,6-cyclization, and deprotonation of the pro-R hydrogen cascade. The structural basis was also investigated by a series of mutagenesis studies. An engineered cell factory for overproducing sphaeroane compounds at the hundred-milligram-per-liter level was achieved.
WOS关键词DITERPENES ; CYCLASES
资助项目Taishan Scholar Project of Shandong Province[tsqn20230623] ; Natural Science Foundation of Shandong Province[ZR2024QB265] ; Key Technology Research and Development Program of Shandong Province[2024CXPT029] ; National Natural Science Foundation of China[22407117] ; Shandong Laboratory Program[SYS202205] ; National Key Research and Development Program of China[2022YFC2804100] ; Shanghai Pujiang Program[23PJ1415300]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001617310300001
出版者AMER CHEMICAL SOC
源URL[http://119.78.100.183/handle/2S10ELR8/321747]  
专题中国科学院上海药物研究所
通讯作者Xu, Zhengren; Xu, Baofu
作者单位1.Bohai Rim Adv Res Inst Drug Discovery, Shandong Lab Yantai Drug Discovery, Yantai 264117, Shandong, Peoples R China
2.Anhui Univ Chinese Med, Hefei 230038, Peoples R China
3.Peking Univ, Sch Pharmaceut Sci, Dept Integrat Chinese & Western Med, Sch Basic Med Sci,State Key Lab Nat & Biomimet Dru, Beijing 100191, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Mat Med, Shanghai 201203, Peoples R China
推荐引用方式
GB/T 7714		 Li, Xin,Liu, Yuanning,Chen, Jiaxing,et al. Discovery, Mechanism, and Bioproduction Studies of a Moss-Derived Microbial-like Terpene Synthase CrMTPSL3 Generating the Tricyclic Sphaeroane Scaffold[J]. ACS CATALYSIS,2025:8.
APA Li, Xin.,Liu, Yuanning.,Chen, Jiaxing.,Wang, Chen.,Chen, Bao.,...&Xu, Baofu.(2025).Discovery, Mechanism, and Bioproduction Studies of a Moss-Derived Microbial-like Terpene Synthase CrMTPSL3 Generating the Tricyclic Sphaeroane Scaffold.ACS CATALYSIS,8.
MLA Li, Xin,et al."Discovery, Mechanism, and Bioproduction Studies of a Moss-Derived Microbial-like Terpene Synthase CrMTPSL3 Generating the Tricyclic Sphaeroane Scaffold".ACS CATALYSIS (2025):8.

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来源：上海药物研究所

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