DNA Framework–Programmed Nanoscale Enzyme Assemblies

作者：Nan Cao, Ruiyan Guo, Ping Song, Shaopeng Wang, Gang Liu, Jiye Shi, Lihua Wang, Min Li, Min Li, Xiaolei Zuo, Xiurong Yang, Chunhai Fan, Mingqiang Li, Mingqiang Li, Yueyue Zhang · 发表于：Nano Letters · 年份：2024 · DOI：10.1021/acs.nanolett.4c01137 · 被引用次数：13 · 研究领域：Advanced biosensing and bioanalysis techniques、DNA and Nucleic Acid Chemistry、Click Chemistry and Applications

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 ∼5.9- and ∼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.