High-Efficient Energy Funneling Based on Electrochemiluminescence Resonance Energy Transfer in Graded-Gap Quantum Dots Bilayers for Immunoassay
High-Efficient Energy Funneling Based on Electrochemiluminescence Resonance Energy Transfer in Graded-Gap Quantum Dots Bilayers for Immunoassay
复制标题
用于免疫测定的分级间隙量子点双层中基于电化学发光共振能量转移的高效能量漏斗
DOI：
10.1021/ac500351d
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发表时间：
2014-04-01
影响因子：
7.4
通讯作者：
Zhu, Jun-Jie
中科院分区：
文献类型：
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作者：
Ji, Jing;He, Li;Zhu, Jun-Jie
观察到梯度间隙CdSeTe@ZnS-SiO2量子点（QD）双层中令人惊讶的电化学发光（ECL）增强效应，并用于创建超灵敏的免疫测定。两种不同尺寸的CdSeTe@ZnS-SiO2量子点被用作供体-受体对，由于它们的可调谐能量和低生物毒性。通过将不同尺寸的CdSeTe @ ZnS-SiO2量子点层层组装到戊二醛去活化的电极上，制备了具有梯度带隙的CdSeTe @ ZnS-SiO2量子点双层结构。受益于渐变能隙量子点双层中的短层间距离和完美的光谱重叠，观察到高效的基于ECL共振能量转移（ECLRET）的能量泛函，其中来自捕获态的激子可以有效地再循环。因此，所观察到的双层的ECL增强是所观察到的参比样品的四倍以上。将该量子点双层膜应用于电化学发光生物传感器中，用于检测癌胚抗原（CEA）。该方法的检出限为0.4 pg mL（-1）CEA，线性范围为1 pg mL（-1）~ 200 ng mL（-1）。这种方法代表了一种新的方法，用于研究和临床应用中的生物分子的通用检测。
A surprising electrochemiluminescence (ECL) enhancement effect in graded-gap CdSeTe@ZnS-SiO2 quantum dot (QD) bilayers was observed and used to create an ultrasensitive immunoassay. CdSeTe@ZnS-SiO2 QDs of two different sizes were used as a donor-acceptor pair, owing to their tunable energy and low biotoxicity. The graded-gap CdSeTe@ZnS-SiO2 QD bilayers were fabricated by layer-by-layer assembly of differently sized CdSeTe@ZnS-SiO2 QDs on a glutaraldehyde-activated electrode. Benefiting from a short interlayer distance and perfect spectral overlap in the graded-gap QD bilayers, highly efficient ECL resonance energy transfer (ECLRET)-based energy funneling was observed, wherein excitons from trapped states could be effectively recycled. Consequently, the observed ECL enhancement for the bilayers was more than four times greater than that observed for reference samples. The graded-gap QD bilayers were utilized in an ECL biosensor for the detection of carcinoembryonic antigen (CEA). The proposed method featured a detection limit of 0.4 pg mL(-1) CEA with a linear calibration range from 1 pg mL(-1) to 200 ng mL(-1). This method represents a novel approach for versatile detection of biomolecules in research and clinical applications.