DNA 四面体纳米结构的门控瞬态耗散二聚化用于程序化 DNA 酶催化,ACS Nano

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DNA 四面体纳米结构的门控瞬态耗散二聚化用于程序化 DNA 酶催化
ACS Nano ( IF 15.8 ) Pub Date : 2022-02-20 , DOI: 10.1021/acsnano.1c06117
Zhenzhen Li ₁ , Jianbang Wang ₁ , Zhixin Zhou ₁ , Michael P O'Hagan ₁ , Itamar Willner ₁

Affiliation

DNA四面体纳米结构的瞬态耗散二聚化和瞬态门控二聚化被引入作为功能模块，以模拟瞬态和门控蛋白质-蛋白质相互作用和紧急蛋白质-蛋白质引导的瞬态催化功能，在自然界中运行。四个四面体被改造以产生功能模块，在预先设计的辅助核酸和切口酶 Nt.BbvCI 的存在下，导致两对四面体的瞬时二聚化。DNA 四面体的动态瞬态形成和消耗之后是由荧光团标记的四面体产生的瞬态 FRET 信号。在四个四面体和两个辅助模块的混合物中整合两种抑制剂，促进瞬态二聚化，导致两种不同的 DNA 四面体二聚体的选择性抑制剂引导的门控瞬时二聚化。DNA四面体的动态瞬态二聚化和门控瞬态二聚化的动力学模型被制定和计算模拟。导出的速率常数允许预测和随后的实验验证系统在不同辅助条件下的性能。此外，通过对四个四面体结构的适当修改，证明了由两对 DNA 四面体二聚体驱动的选择性瞬时催化功能的触发门控出现。导出的速率常数允许预测和随后的实验验证系统在不同辅助条件下的性能。此外，通过对四个四面体结构的适当修改，证明了由两对 DNA 四面体二聚体驱动的选择性瞬时催化功能的触发门控出现。导出的速率常数允许预测和随后的实验验证系统在不同辅助条件下的性能。此外，通过对四个四面体结构的适当修改，证明了由两对 DNA 四面体二聚体驱动的选择性瞬时催化功能的触发门控出现。

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Gated Transient Dissipative Dimerization of DNA Tetrahedra Nanostructures for Programmed DNAzymes Catalysis

Transient dissipative dimerization and transient gated dimerization of DNA tetrahedra nanostructures are introduced as functional modules to emulate transient and gated protein–protein interactions and emergent protein–protein guided transient catalytic functions, operating in nature. Four tetrahedra are engineered to yield functional modules that, in the presence of pre-engineered auxiliary nucleic acids and the nicking enzyme Nt.BbvCI, lead to the fueled transient dimerization of two pairs of tetrahedra. The dynamic transient formation and depletion of DNA tetrahedra are followed by transient FRET signals generated by fluorophore-labeled tetrahedra. The integration of two inhibitors within the mixture of the four tetrahedra and two auxiliary modules, fueling the transient dimerization, results in selective inhibitor-guided gated transient dimerization of two different DNA tetrahedra dimers. Kinetic models for the dynamic transient dimerization and gated transient dimerization of the DNA tetrahedra are formulated and computationally simulated. The derived rate-constants allow the prediction and subsequent experimental validation of the performance of the systems under different auxiliary conditions. In addition, by appropriate modification of the four tetrahedra structures, the triggered gated emergence of selective transient catalytic functions driven by the two pairs of DNA tetrahedra dimers is demonstrated.

更新日期：2022-02-20

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