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基于超声作用下活性氧加速生成的自增强电化学发光成像系统

Self-Enhanced Electrochemiluminescence Imaging System Based on the Accelerated Generation of ROS under Ultrasound.

作者信息

Zhu Hui, Zhou Jia-Lin, Ma Cheng, Jiang Dechen, Cao Yue, Zhu Jun-Jie

机构信息

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, P. R. China.

出版信息

Anal Chem. 2023 Aug 1;95(30):11526-11534. doi: 10.1021/acs.analchem.3c02183. Epub 2023 Jul 18.

Abstract

Electrochemiluminescence (ECL) imaging, as an optical technology, has been developed at full tilt in the field of life science and nanomaterials. However, the relatively low ECL intensity or the high co-reactant concentration needed in the electrochemical reaction blocks its practical application. Here, we developed an ECL imaging system based on the rGO-TiO composite material, where the co-reactant, reactive oxygen species (ROS), is generated in situ under the synergetic effect of of ultrasound (US) and electric irradiation. The rGO-TiO composites facilitate the separation of electron (e) and hole (h) pairs and inhibit recombination triggered by external US irradiation due to the high electroconductivity of rGO and oxygen-deficient structures of TiO, thus significantly boosting ROS generation. Furthermore, the increased defects on rGO accelerate the electron transfer rate, improving the electrocatalytic performance of the composite and forming more ROS. This high ultrasonic-electric synergistic efficacy is demonstrated through the enhancement of photon emission. Compared with the luminescence intensity triggered by US irradiation and electric field, an enhancement of ∼20-fold and 10-fold of the US combined with electric field-triggered emission is observed from this composite. Under the optimized conditions, using dopamine (DA) as a model target, the sensitivity of the US combined ECL strategy for detection of DA is two orders of magnitude higher than that of the ECL method. The successful detection of DA at low concentrations makes us believe that this strategy provides the possibility of applying ECL imaging for cellular single-molecule analysis and cancer therapy.

摘要

电化学发光(ECL)成像作为一种光学技术,已在生命科学和纳米材料领域得到充分发展。然而,电化学反应中相对较低的ECL强度或所需的高共反应物浓度阻碍了其实际应用。在此,我们开发了一种基于rGO-TiO复合材料的ECL成像系统,其中共反应物活性氧(ROS)在超声(US)和电辐射的协同作用下原位生成。rGO-TiO复合材料促进了电子(e)和空穴(h)对的分离,并由于rGO的高导电性和TiO的缺氧结构抑制了外部US辐射引发的复合,从而显著促进了ROS的生成。此外,rGO上增加的缺陷加速了电子转移速率,提高了复合材料的电催化性能并形成了更多的ROS。这种高超声-电协同效应通过光子发射的增强得到证明。与US辐射和电场引发的发光强度相比,该复合材料在US与电场联合触发发射时观察到增强了约20倍和10倍。在优化条件下,以多巴胺(DA)为模型目标,US联合ECL策略检测DA的灵敏度比ECL方法高两个数量级。低浓度DA的成功检测使我们相信该策略为将ECL成像应用于细胞单分子分析和癌症治疗提供了可能性。

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