DNA Framework-Programmed Nanoscale Enzyme Assemblies

被引：5

作者：

Cao, Nan ^{[1
,2
,3
,4
]}

Guo, Ruiyan ^{[1
,2
,5
]}

Song, Ping ^{[6
]}

Wang, Shaopeng ^{[1
,2
]}

Liu, Gang ^{[2
,5
]}

Shi, Jiye ^{[2
,7
]}

Wang, Lihua ^{[2
,7
]}

Li, Min ^{[1
,2
]}

Zuo, Xiaolei ^{[1
,2
]}

Yang, Xiurong ^{[3
,4
,8
]}

Fan, Chunhai ^{[1
,2
,3
,4
]}

Li, Mingqiang ^{[1
,2
,3
,4
]}

Zhang, Yueyue ^{[1
,2
]}

机构：

[1] Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200127, Peoples R China

[2] Shanghai Jiao Tong Univ, Renji Hosp, Inst Mol Med, Sch Med,Shanghai Key Lab Nucl Acid Chem & Nanomed, Shanghai 200127, Peoples R China

[3] Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Shanghai 200240, Peoples R China

[4] Shanghai Jiao Tong Univ, Natl Ctr Translat Med, Shanghai 200240, Peoples R China

[5] Shanghai Inst Measurement & Testing Technol, Key Lab Bioanal & Metrol State Market Regulat, Shanghai 201203, Peoples R China

[6] Shanghai Jiao Tong Univ, Sch Biomed Engn, State Key Lab Oncogenes & Related Genes, Shanghai 200030, Peoples R China

[7] Chinese Acad Sci, Shanghai Inst Appl Phys, Div Phys Biol, CAS Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China

[8] Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Jilin, Peoples R China

来源：

NANO LETTERS | 2024年 / 24卷 / 15期

基金：

上海市自然科学基金;

关键词：

DNA Framework; Nanoscale Phase Separation; 3D Multienzyme Assemblies; Enzyme Cascade; ActivityEnhancement; MULTIENZYME COMPLEXES; CASCADE; CATALYSIS; DRIVEN; DESIGN;

D O I：

10.1021/acs.nanolett.4c01137

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Multienzyme assemblies mediated by multivalent interaction play a crucial role in cellular processes. However, the three-dimensional (3D) programming of an enzyme complex with defined enzyme activity in vitro remains unexplored, primarily owing to limitations in precisely controlling the spatial topological configuration. Herein, we introduce a nanoscale 3D enzyme assembly using a tetrahedral DNA framework (TDF), enabling the replication of spatial topological configuration and maintenance of an identical edge-to-edge distance akin to natural enzymes. Our results demonstrate that 3D nanoscale enzyme assemblies in both two-enzyme systems (glucose oxidase (GOx)/horseradish peroxidase (HRP)) and three-enzyme systems (amylglucosidase (AGO)/GOx/HRP) lead to enhanced cascade catalytic activity compared to the low-dimensional structure, resulting in similar to 5.9- and similar to 7.7-fold enhancements over homogeneous diffusional mixtures of free enzymes, respectively. Furthermore, we demonstrate the enzyme assemblies for the detection of the metabolism biomarkers creatinine and creatine, achieving a low limit of detection, high sensitivity, and broad detection range.

引用

页码：4682 / 4690

页数：9

共 57 条

[1] Pervasive cooperative mutational effects on multiple catalytic enzyme traits emerge via long-range conformational dynamics [J].