Yang Huan, Wang Huan, Wang Po, Feng Qiumei
School of Chemistry and Materials Science, Jiangsu Normal University, Xuzhou 221116, China.
ACS Appl Mater Interfaces. 2025 Jan 15;17(2):3052-3061. doi: 10.1021/acsami.4c18752. Epub 2025 Jan 6.
Sensitive and accurate determination of acetamiprid is highly desirable for guaranteeing food safety. In this Letter, an energy-transfer-based dual-mode biosensor was developed using zinc-based metal-organic frameworks (Zn-MOFs) acting as both photoelectrochemical (PEC) and electrochemiluminescent (ECL) donors and Pt@CuO cubic nanocrystals (CNs) as the energy acceptor for detecting acetamiprid. By integration of aptamer recognition with two-step DNA circuit amplification (entropy-driven DNA cycle and DNA walker), the detection of acetamiprid was converted into the assay of abundant intermediate DNA strands. With the help of nicking endonuclease, a large number of single-stranded DNAs was generated on the surface of Zn-MOFs, which were used as multifunctional PEC and ECL substrates. Through competitive hybridization, Pt@CuO CNs as broad-spectrum quenchers were introduced, thereby enabling changes in the PEC and ECL responses for acetamiprid quantitation. The experimental results proved that the combination of energy transfer, two-step DNA circuit amplification, and dual-mode sensing strategy achieved the sensitive and accurate analysis of acetamiprid, with low detection limits of 20.2 fM (PEC mode) and 17.5 fM (ECL mode) within a wide range from 0 to 1 × 10 M. The excellent specificity, reproducibility, and practicality confirmed the potential application of the biosensor for pesticide-related food safety.
为保障食品安全，对啶虫脒进行灵敏且准确的测定至关重要。在本信函中，开发了一种基于能量转移的双模式生物传感器，该传感器使用锌基金属有机框架（Zn-MOFs）作为光电化学（PEC）和电化学发光（ECL）供体，并使用Pt@CuO立方纳米晶体（CNs）作为能量受体来检测啶虫脒。通过将适体识别与两步DNA电路扩增（熵驱动DNA循环和DNA步行器）相结合，啶虫脒的检测被转化为对大量中间DNA链的测定。在切口内切酶的帮助下，在Zn-MOFs表面产生了大量单链DNA，这些单链DNA被用作多功能PEC和ECL底物。通过竞争性杂交，引入了作为广谱猝灭剂的Pt@CuO CNs，从而实现了用于啶虫脒定量的PEC和ECL响应变化。实验结果证明，能量转移、两步DNA电路扩增和双模式传感策略的结合实现了对啶虫脒的灵敏且准确的分析，在0至1×10 M的宽范围内检测限低至20.2 fM（PEC模式）和17.5 fM（ECL模式）。优异的特异性、重现性和实用性证实了该生物传感器在农药相关食品安全方面的潜在应用。
