基于超声下ROS加速产生的自增强电化学发光成像系统,Analytical Chemistry

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基于超声下ROS加速产生的自增强电化学发光成像系统
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-07-18 , DOI: 10.1021/acs.analchem.3c02183
Hui Zhu ₁ , Jia-Lin Zhou ₁ , Cheng Ma _{1,

2} , Dechen Jiang ₁ , Yue Cao _{1,

3} , Jun-Jie Zhu ₁

Affiliation

电化学发光（ECL）成像作为一种光学技术，在生命科学和纳米材料领域得到了全面发展。然而，电化学反应所需的相对较低的ECL强度或较高的共反应物浓度阻碍了其实际应用。在这里，我们开发了一种基于rGO-TiO _{2– x}复合材料的ECL成像系统，其中在超声波（US）和电辐射的协同作用下原位产生共反应物活性氧（ROS）。由于rGO的高导电性和TiO 2 的缺氧结构，rGO _- TiO _{2– x}^{复合材料促进了电子（e -}）和空穴（h ⁺ ）对的分离，并抑制了由外部US辐射引发的复合，从而显着促进ROS的产生。此外，rGO上缺陷的增加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更多的ROS。这种高超声电协同功效是通过光子发射的增强得到证明的。与US辐射和电场触发的发光强度相比，从该复合材料中观察到US与电场触发发射相结合的发光强度分别增强了约20倍和10倍。在优化条件下，以多巴胺（DA）为模型靶点，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应用ECL成像进行细胞单分子分析和癌症治疗提供了可能性。

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

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_2–x 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_2–x 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 TiO₂, 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.

更新日期：2023-07-18

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