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pH-controlled DNAzymes： Rational design and their applications in DNA-machinery devices

Nano Research 2016年第10期9卷 3084-3092页

作者： Yuqi Chen Yanyan Song Zhiyong He Zijing Wang Wenting Liu FuanWang Xiaolian Zhang Xiang Zhou College of Chemistry and Molecular Sciences The Institute for Advanced Studies Wuhan University Wuhan 430072 China School of Medicine Wuhan University Wuhan 430071 China

The availability and reliability of strategies for molecular biosensing over a finely adjustable dynamic range is essential to enhance the understanding and control of vital biological process. To expand the versatility and utility of nucleic acid- related enzymes, we demonstrated a rational approach to acquiring tunable, pH-dependent deoxyribozymes （DNAzymes） with catalytic activities and response sensitivities that can be tuned through a simple change in solution pH. To do this, we capitalized upon the pH dependence of Hoogsteen interactions and designed i-motif- and triplex-based DNAzymes that can be finely regulated with high precision over a physiologically relevant pH interval. The modified DNAzymes are dependent upon pH for efficient cleavage of substrates, and their catalytic performance can be tuned by regulating the sequence of inserted i-motif/triplex structures. The principle of tunable, pH-dependent DNAzymes provides the opportunity to engineer pH-controlled DNA-machinery devices with unprecedented sensitivity to pH changes. For example, we constructed a DNA-walker device, the stepping rate of which could be adjusted by simply modulating solution pH within an interval of 5.6 to 7.4, as well as a DNA tetrahedron that can be opened at pH 6.4 and kept closed at pH 7.4. The potential of this approach is not limited to serve as pH-dependent devices, but rather may be combined with other elements to expand their practical usefulness.

关键词： pH iMNAzyme tnazyme DNA walker DNA tetrahedron

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