Hyun Shin , Jun-Young Cho , Boyoung Y. Park , Cheulhee Jung
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引用次数: 0
Abstract
DNAzymes play a crucial role in biosensors for signal detection, but specific structures are required for diagnostic applications, complicating their design. This study reports a novel approach to the development of DNAzymes by incorporating sulfur atoms into nucleic acids via phosphorothioate (PS) bonds. Unlike traditional DNAzymes that rely on specific structures such as G-quadruplexes, this approach leads to high enzymatic activity without structural constraints. Computational analysis reveals that the change in the electron density of the nucleobases due to PS modification enhances interactions within the DNAzyme-H2O2-hemin complex, accelerating the rate-determining step and improving enzymatic activity. Systematic guidelines for the development of non-sequence constrained DNAzymes are provided by investigating the effect of the number of PS modifications, the length of the DNA, and various nucleobase combinations. α-thio-dNTP, a monomer containing PS, exhibits no observable enzymatic activity, but enzymatic activity is recorded for single-stranded DNA (ssDNA) containing PS. However, when the ssDNA is transformed into double-stranded DNA (dsDNA), the bases that react with hemin are blocked by hydrogen bonding, reducing enzymatic activity. An enzymogenic signaling system that differentiates between ssDNA and dsDNA is subsequently developed for sequence-specific colorimetric detection, demonstrating significant promise for overcoming the limitations of conventional DNAzymes in molecular diagnosis.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.