Development of Hollow Electrochemiluminescent Nanocubes Combined with a Multisite-Anchored DNA Nanomachine for Mycotoxin Detection
Development of Hollow Electrochemiluminescent Nanocubes Combined with a Multisite-Anchored DNA Nanomachine for Mycotoxin Detection
复制标题
开发空心电化学发光纳米立方体与多位点锚定 DNA 纳米机器相结合用于霉菌毒素检测
DOI：
10.1021/acs.analchem.1c00446
复制
发表时间：
2021
影响因子：
7.4
通讯作者：
Ying Zhuo
中科院分区：
文献类型：
--
作者：
Xia Zhong;Shan-Shan Yang;Ni Liao;Ruo Yuan;Ying Zhuo
多环芳烃（PAHs）具有量子效率高、制备成本低等优点，被认为是一种很有前途的电致发光材料。尽管纯PAH微晶（如红荧烯微晶，Rub MCs）的电致发光特性已受到广泛关注，但如何控制其形貌和尺寸以降低内滤光效应仍是一个挑战。本文中，通过原位氧化还原沉积方法制备了钯纳米颗粒官能化的中空PAH-金属纳米立方体的先进ECL发射体（所得纳米复合材料缩写为Pd-Rub-Ag@Au纳米立方体）。以Ag@ Au纳米立方体为模板，红荧烯阳离子自由基（Rub·+）为还原剂，制备了红荧烯修饰的Ag @Au纳米立方体（Rub-Ag@Au nanocubes），并在Rub-Ag@Au纳米立方体表面原位还原了Pd纳米粒子（PdNPs）。令人印象深刻的是，与Rub MCs相比，Pd-Rub-Ag@Au纳米立方体在水介质中显示出均匀的尺寸和显著增强的ECL效率和强度。作为概念验证，构建了基于Pd-Rub-Ag@Au纳米立方体的电化学发光生物传感平台与多位点锚定DNA纳米机器相结合，用于赭曲霉毒素A（OTA，一种真菌毒素）的检测。覆盖有高密度识别序列的DNA纳米机器可以在传感平台上进行支点介导的链置换扩增，大大提高了运动效率和速度。由于Pd-Rub-Ag@Au纳米立方体的优异性能和DNA纳米机器的高识别效率，该生物传感器用于OTA检测的检测限可达4.7 fg/mL，检测范围为0.01 ~ 100 pg/mL，为多环芳烃的进一步应用提供了一种巧妙的方法。
Polycyclic aromatic hydrocarbons (PAHs) are regarded as promising electrochemiluminescent (ECL) emitters owing to their high quantum efficiency and inexpensive production. Despite the fact that the ECL properties of the pure PAH microcrystal (such as rubrene microcrystals, Rub MCs) have gained extensive attention, it is a challenge in controlling the morphology and size to reduce the inner filter effect. Herein, an advanced ECL emitter of palladium nanoparticle-functionalized hollow PAH-metal nanocubes was prepared by an in situ redox deposition method (the resultant nanocomposites were abbreviated as Pd-Rub-Ag@Au nanocubes). Specifically, the rubrene-decorated Ag@Au nanocubes (Rub-Ag@Au nanocubes) were prepared using the Ag@Au nanocubes as a template and a rubrene cation radical (Rub•+) as a reductant, and then Pd nanoparticles (Pd NPs) were in situ reduced on the surface of Rub-Ag@Au nanocubes. Impressively, compared with the Rub MCs, Pd-Rub-Ag@Au nanocubes showed uniform size and significantly enhanced ECL efficiency and intensity in the aqueous media. As a proof-of-concept, the Pd-Rub-Ag@Au nanocube-based ECL biosensing platform combined with a multisite-anchored DNA nanomachine was constructed for ochratoxin A (OTA, a type of mycotoxin) detection. The DNA nanomachine covered with high-density recognizing sequences could operate toehold-mediated strand displacement amplification on the sensing platform and promote the movement efficiency and velocity greatly. Due to the advanced performance of Pd-Rub-Ag@Au nanocubes and high recognition efficiency of the DNA nanomachine, the proposed biosensor for OTA detection can achieve a detection limit of 4.7 fg/mL ranging from 0.01 to 100 pg/mL, which offers an ingenious method for the further application of PAHs.