Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis

doi:10.1021/jacs.4c06171

	Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis
	Li, Yinhao 1,4; Ding, Jiawang1,4 ; Qin, Wei1,2,3,4
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
	2024-07-29
页码	9
DOI	10.1021/jacs.4c06171
通讯作者	Ding, Jiawang([email protected]) ; Qin, Wei([email protected])
英文摘要	Natural enzymes with enhanced catalytic activity and selectivity have long been studied by tuning the microenvironment around the active site, but how to modulate the active-site electric field in a simple fashion remains challenging. Here, we demonstrate that microdroplets as a simple yet versatile reactor can enhance the electric field at the active site of an enzyme. By using horseradish peroxidase as a model, improved selectivity in microdroplet-mediated enzyme catalysis can be obtained. Quantum mechanical/molecular dynamics calculations and vibrational Stark spectroscopy reveal that the electric field at the microdroplet interface can influence the electrostatic preorganization and orientation of the enzyme to enhance its internal electric field. As a result, the free energies of the substrate and heme can be tuned by the internal electric field, thereby changing its catalytic reaction pathway for a classical substrate, 3,3 ',5,5 '-tetramethylbenzidine, and enabling selective C-N additions for specific substrates. This finding provides a green, simple, and effective way to modulate enzyme-catalyzed reactions and holds promise for a broad spectrum of biosensing and biosynthesis applications.
资助机构	National Natural Science Foundation of China ; Taishan Scholar Program of Shandong Province ; Special Fund for the Scholar Program of Yantai and Shandong Province ; Key Development Project of Centre for Ocean Mega-Research of Science, Chinese Academy of Sciences ; Seed Project of Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences
收录类别	SCI
语种	英语
关键词[WOS]	ELECTRIC-FIELDS ; ELECTROSTATIC CATALYSIS ; PEROXIDASE ; OXIDATION ; RADICALS
研究领域[WOS]	Chemistry
WOS记录号	WOS:001280421000001
引用统计	被引频次：1[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.yic.ac.cn/handle/133337/35670
专题	中国科学院海岸带环境过程与生态修复重点实验室中国科学院海岸带环境过程与生态修复重点实验室_海岸带环境过程实验室
通讯作者	Ding, Jiawang; Qin, Wei
作者单位	1.Chinese Acad Sci, CAS Key Lab Coastal Environm Proc & Ecol Remediat, Shandong Key Lab Coastal Environm Proc, Yantai Inst Coastal Zone Res YIC,YICCAS, Yantai 264003, Shandong, Peoples R China 2.Qingdao Marine Sci & Technol Ctr, Lab Marine Biol & Biotechnol, Qingdao 266237, Shandong, Peoples R China 3.Chinese Acad Sci, Ctr Ocean Mega Sci, Qingdao 266071, Shandong, Peoples R China 4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Li, Yinhao,Ding, Jiawang,Qin, Wei. Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024:9.
APA	Li, Yinhao,Ding, Jiawang,&Qin, Wei.(2024).Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,9.
MLA	Li, Yinhao,et al."Enhanced Selectivity in Microdroplet-Mediated Enzyme Catalysis".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2024):9.