适体
电场
检出限
电化学
化学
二茂铁
纳米技术
组合化学
材料科学
色谱法
电极
物理
分子生物学
量子力学
物理化学
生物
作者
Chang Liu,Yuan Wang,Yuye Li,Suci Meng,Wenjia Li,Dong Liu,Tianyan You
标识
DOI:10.1016/j.scitotenv.2023.166407
摘要
Aptamers with strong affinity to heavy metal ions (HMIs) allow fabrication of electrochemical sensors with high selectivity and sensitivity, while controllable regulation of aptamer-HMI recognition at the sensing interface, which is vital for better analytical performance, remains challenging. Here, an electric field-based strategy for engineering an aptasensing interface was proposed to realize the specific preconcentration and accurate detection of mercury (Hg2+) and lead (Pb2+) ions with a ratiometric electrochemical sensor. The working principle is to apply an electric field to drive HMIs to approach the aptamer and retain the orientation of the DNA structure. Anthraquinone-2-carboxylic acid (AQ)-labeled complementary DNA was designed to simultaneously bind a ferrocene (Fc)-labeled aptamer for Hg2+ and a methylene blue (MB)-labeled aptamer for Pb2+, and the sensing interface was fabricated with this presynthesized DNA structure. For preconcentration, an electric field of 3.0 V pushed HMIs to approach the aptamer and retained the orientation of DNA to favor the following recognition; for detection, the oriented DNA in 2.5 V electric field offered a stable current of AQ as a reference. In this way, currents of AQ, Fc and MB were used to produce ratiometric signals of IAQ/IFc and IAQ/IMB for Hg2+ and Pb2+, respectively. Such a strategy allowed the simultaneous detection of Hg2+ and Pb2+ within 30 min with detection limits of 0.69 pM and 0.093 pM, respectively. The aptasensor was applied for soil, water, and crayfish analysis in paddy fields. The electric field-enabled strategy offers a new way to fabricate high-performance electrochemical aptasensor for HMIs detection.
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