化学
核酸
分析物
纳米技术
脱氧核酶
核酸检测
反式激活crRNA
正交性
灵敏度(控制系统)
核酸定量
DNA
组合化学
计算生物学
副溶血性弧菌
寡核苷酸
分子信标
清脆的
DNA纳米技术
作者
Shoujia Lin,Xiangbin Chen,Ziyue Lang,Bozhi Lu,Yanwei Jia,Huangxian Ju,Hongmei Cao
标识
DOI:10.1021/acs.analchem.6c04985
摘要
CRISPR/Cas12a has emerged as an important platform for nucleic acid analysis, yet limited catalytic turnover and intrinsic nucleic acid specificity constrain its sensitivity and analyte scope. Herein, a tight-locking and high-gain Cas12a-driven strand displacement amplification (CSDA) molecular circuit is developed as a versatile socket without preamplification for programmable sensing of nucleic acid and non-nucleic acid analytes. CSDA relies on an RNA-DNA three-strand hairpin (RD-TSH) switch containing a 2-nt mismatch. RD-TSH suppresses nonspecific amplification and unintended Cas12a self-activation to ensure tight locking. Screening the number of mismatched bases in RD-TSH and molecular-level mechanistic analyses reveal a DNA breathing-driven two-step unlocking mechanism. Only complete unlocking triggers autocatalytic CSDA, allowing high-gain amplification. The sequence-independent unlocking of RD-TSH confers high orthogonality to CSDA, enabling target-specific modules to be coupled to the CSDA socket as interchangeable plugs via programmable crRNA guides, thus achieving universal detection of both nucleic and non-nucleic analytes. Using Vibrio parahaemolyticus DNA, thermostable direct hemolysin, and aflatoxin B1 as representative targets, CSDA achieved ultrasensitive detection in complex matrices with sensitivity improvements of over 5 orders of magnitude, 42-fold, and 602-fold, respectively. This plug-and-play architecture establishes CSDA as a broadly adaptable and ultrasensitive CRISPR/Cas12a sensing socket, providing a general route toward programmable sensing of diverse analyte classes and a promising strategy for more accurate integrated multitarget analytical platforms.
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