为在一个细微地可调节的动态范围上的分子的 biosensing 的策略的可获得性和可靠性是必要的提高重要生物过程的理解和控制。扩展 nucleic acidrelated 酶的通用性和实用程序,我们表明了一条合理途径到与能在解决方案 pH 通过一个简单变化被调节的催化活动和反应敏感获得悦耳的、 pH 依赖的 deoxyribozymes (DNAzymes ) 。做这,我们在 Hoogsteen 相互作用的 pH 依赖之上大写并且设计了能细微地在生理地相关的 pH 间隔上与高精确被调整的 i-motif- 和三重底的 DNAzymes。修改 DNAzymes 依赖于为底层的有效劈开的 pH,并且他们的催化表演能被调整插入的 i-motif/triplex 结构的顺序调节。悦耳的、 pH 依赖的 DNAzymes 的原则提供机会与崭新的敏感设计控制 pH 的 DNA 机械设备到 pH 变化。例如,我们构造了一台 DNA 行人设备,哪个能被调整由的走的率简单地在 5.6 ~ 7.4 的间隔以内的 modulating 答案 pH,以及能在 pH 被打开的一个 DNA 四面体 6.4 并且在 pH 密切注视 7.4。这条途径的潜力没被限制用作 pH 依赖的设备,但是可以相当与另外的元素被相结合扩展他们的实际实用性。
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.