Tram Kha, Xia Jiaji, Gysbers Rachel, Li Yingfu
Department of Chemistry and Chemical Biology, McMaster University, Hamilton, Ontario, Canada.
Department of Biochemistry and Biomedical Sciences, McMaster University, Hamilton, Ontario, Canada.
PLoS One. 2015 May 6;10(5):e0126402. doi: 10.1371/journal.pone.0126402. eCollection 2015.
Many DNAzymes have been isolated from synthetic DNA pools to cleave natural RNA (D-RNA) substrates and some have been utilized for the design of aptazyme biosensors for bioanalytical applications. Even though these biosensors perform well in simple sample matrices, they do not function effectively in complex biological samples due to ubiquitous RNases that can efficiently cleave D-RNA substrates. To overcome this issue, we set out to develop DNAzymes that cleave L-RNA, the enantiomer of D-RNA, which is known to be completely resistant to RNases. Through in vitro selection we isolated three L-RNA-cleaving DNAzymes from a random-sequence DNA pool. The most active DNAzyme exhibits a catalytic rate constant ~3 min-1 and has a structure that contains a kissing loop, a structural motif that has never been observed with D-RNA-cleaving DNAzymes. Furthermore we have used this DNAzyme and a well-known ATP-binding DNA aptamer to construct an aptazyme sensor and demonstrated that this biosensor can achieve ATP detection in biological samples that contain RNases. The current work lays the foundation for exploring RNA-cleaving DNAzymes for engineering biosensors that are compatible with complex biological samples.
许多脱氧核酶已从合成DNA文库中分离出来,用于切割天然RNA(D-RNA)底物,其中一些已被用于设计适体酶生物传感器,用于生物分析应用。尽管这些生物传感器在简单的样品基质中表现良好,但由于普遍存在的核糖核酸酶能够有效切割D-RNA底物,它们在复杂生物样品中无法有效发挥作用。为了克服这个问题,我们着手开发能够切割D-RNA对映体L-RNA的脱氧核酶,已知L-RNA对核糖核酸酶具有完全抗性。通过体外筛选,我们从随机序列DNA文库中分离出三种切割L-RNA的脱氧核酶。活性最高的脱氧核酶表现出约3 min-1的催化速率常数,其结构包含一个吻环,这是一种在切割D-RNA的脱氧核酶中从未观察到的结构基序。此外,我们使用这种脱氧核酶和一种著名的ATP结合DNA适体构建了一种适体酶传感器,并证明这种生物传感器能够在含有核糖核酸酶的生物样品中实现ATP检测。目前的工作为探索用于构建与复杂生物样品兼容的生物传感器的RNA切割脱氧核酶奠定了基础。