期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 30, 页码 13526-13537出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c02884
关键词
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资金
- National Key R & D Program of China [2021YFC2301100]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB30000000]
- National Natural Science Foundation of China [61890940]
- Chongqing Bayu Scholar Program [DP2020036]
- China Postdoctoral Science Foundation [2019M661353]
- National Postdoctoral Program for Innovative Talents [BX20190072]
- Fudan University
In this study, a self-actuated molecular-electrochemical system was proposed to achieve controllable and intelligent modulation of the sensing process. By modifying tentacles and trunks on a graphene microelectrode, the system can efficiently analyze a small amount of biomarkers in unamplified samples and shows high overall agreement with reverse transcription-polymerase chain reaction results. A portable prototype based on this system was fabricated, demonstrating great potential for future applications.
The existing electrochemical biosensors lack controllable and intelligent merit to modulate the sensing process upon external stimulus, leading to challenges in analyzing a few copies of biomarkers in unamplified samples. Here, we present a self-actuated molecular-electrochemical system that consists of a tentacle and a trunk modification on a graphene microelectrode. The tentacle that contains a probe and an electrochemical label keeps an upright orientation, which increases recognition efficiency while decreasing the pseudosignal. Once the nucleic acids are recognized, the tentacles nearby along with the labels are spontaneously actuated downward, generating electrochemical responses under square wave voltammetry. Thus, it detects unamplified SARS-CoV-2 RNAs within 1 min down to 4 copies in 80 mu L, 2-6 orders of magnitude lower than those of other electrochemical assays. Double-blind testing and 10-in-1 pooled testing of nasopharyngeal samples yield high overall agreement with reverse transcription-polymerase chain reaction results. We fabricate a portable prototype based on this system, showing great potential for future applications.
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