期刊
ANALYTICAL CHEMISTRY
卷 91, 期 19, 页码 12468-12475出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.9b03151
关键词
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资金
- Chongqing Research Program of Basic Research and Frontier Technology [cstc2018jcy-jA0797]
- Fundamental Research Funds for the Central Universities [XDJK2019B022, SWU117045, XDJK2018C041]
- National Natural Science Foundation (NNSF) of China [51473136, 21575116]
In this work, hydrazine-functionalized perylene diimide derivative supramolecular (HPDS), a novel self-enhanced donor-acceptor-donor (D-A-D) type aggregates with excellent photoelectric activity, was synthesized by a facile one-pot green route and further applied in construction of coreactant-free photoelectrochemical (PEC) biosensor for ultrasensitive DNA assay. Impressively, the HPDS formed by D-A-D units not only possessed effectively shorted electrontransfer path between donor and acceptor, but also presented a desiring aggregate state via the pi-pi stacking of perylene core and hydrogen bonding of the terminal moiety, thereby acquiring a high density electron flow for generating the extremely high PEC signal. Experimental data showed that the well film-formed HPDS aggregate could produce an exciting photocurrent intensity about 6-fold stronger than that of precursor perylene dianhydride with donor N2H4 in detection buffer and even 12-fold than that of perylene dianhydride only. In this respect, the resultant HPDS aggregate as a novel self-enhanced PEC signal tag was adopted to fabricate the coreactant-free PEC biosensor with the help of target dual-recycling-induced bipedal walker cascade amplification strategy for ultrasensitive DNA (a fragment of TP53 gene) assay. The proposed biosensor showed a high sensitivity with a low detection limit down to femtomole level, providing a new avenue for sensitive bioanalysis and clinical diagnosis.
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