期刊
ACS APPLIED NANO MATERIALS
卷 4, 期 9, 页码 8998-9007出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c01585
关键词
WS2/Bi/BiOBr nanocomposites; 5-formyluracil; signal amplification; photoelectrochemical biosensor; hemin/G-quadruplex; epigenetic modification
资金
- Outstanding Youth Innovation Team of University in Shandong Province [2019KJC019]
- Key Research and Development (Public Welfare) Project of Shandong Province [2019GSF107023]
- National Natural Science Foundation of China [21775090, 41807484, 41977345, 42077363]
The study developed a photoelectrochemical biosensor based on WS2/Bi/BiOBr nanocomposites, black TiO2 (b-TiO2), and hemin/G-quadruplex for the highly sensitive and selective detection of 5-formyluracil-2'-deoxyuridine-5'-triphosphate (5fdUTP). The biosensor showed a linear range of 0.005-500 nM and a detection limit of 1.53 pM, with enhanced PEC response by the hemin/G-quadruplex structure. The method exhibited optimistic selectivity through precision and accuracy evaluation with standard addition recovery experiments.
5-Formyluracil (5fU) is considered an important epigenetic modification agent involved in gene regulation, cell differentiation, and development. 5fU exists in many cells and tissues but is highly similar to the structure of 5-formylcytosine (SfC) and is less abundant in genome. Therefore, the development of a rapid, sensitive, and highly selective method to detect 5fU is desired. In this study, a photoelectrochemical biosensor based on WS2/Bi/BiOBr nanocomposites, black TiO2 (b-TiO2), and hemin/G-quadruplex was described, which was found to be highly sensitive and selective for 5-formyluracil-2'-deoxyuridine-5'-triphosphate (5fdUTP) detection. WS2/Bi/BiOBr was first employed as a photosensitive material, and 3,4-diaminobenzoic acid (DABA) was adopted as a 5fdUTP recognition and capture reagent, where DABA was captured by polyethylene polyamine through covalent reaction to form a stable amid bond. Then, a benzimidazole bond was formed between DABA and -CHO of 5fdUTP, and 5fdUTP was selectively captured on the electrode. Using b-TiO2 as a cross-linker, a guanine-rich ssDNA sequence was further immobilized on the electrode surface by covalent reaction with the 5fdUTP phosphate group. With the assistance of IC and hemin, the hemin/G-quadruplex structure was formed on the electrode. The hemin molecules in the structure of hemin/G-quadruplex obviously enhanced the PEC response of the biosensor for detecting 5fdUTP, with a linear range of 0.005-500 nM and a detection limit of 1.53 pM (S/N = 3). In addition, this method exhibits optimistic selectivity. The precision and accuracy of this method were evaluated by studying the content of 5fdUTP in genome DNA of crop tissues with standard addition recovery experiments.
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