全光电化学发光,Journal of the American Chemical Society

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全光电化学发光
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-07-27 , DOI: 10.1021/jacs.3c05856
Yiran Zhao ₁ , Julie Descamps ₂ , Nour Al Hoda Al Bast ₃ , Marcos Duque ₄ , Jaume Esteve ₄ , Borja Sepulveda ₄ , Gabriel Loget _{1,

5} , Neso Sojic ₂

Affiliation

电化学发光（ECL）广泛应用于医学诊断和成像。尽管其具有卓越的分析性能，但该技术本质上仍然受到对外部电源和用于电极连接的电线的基本需求的限制。在这里，我们报告了一种电气自主解决方案，通过设计基于用催化涂层改性的纳米结构硅光伏结的完全集成的全光学无线单片光电化学装置，导致范式改变。在可见光到近红外光照射下，光生空穴引起 ECL 试剂氧化，从而发射可见 ECL 光子。蓝色 ECL 发射很容易用肉眼观察并用智能手机记录。因此引入了一种新的发光方案，其中通过中间电化学过程，ECL 发射能量 (2.82 eV) 高于激发能量 (1.18 eV)。此外，通过光学显微镜绘制的光电化学活性图揭示了纳米尺度的少数载流子界面转移机制。这一突破为推广 ECL 提供了一种全光学策略，无需电化学设置、电极、接线限制和特定的电化学知识。迄今为止报道的这种最简单的 ECL 配置为开发成像和无线生物分析系统（例如便携式护理点传感设备）提供了新的机会。

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All-Optical Electrochemiluminescence

Electrochemiluminescence (ECL) is widely employed for medical diagnosis and imaging. Despite its remarkable analytical performances, the technique remains intrinsically limited by the essential need for an external power supply and electrical wires for electrode connections. Here, we report an electrically autonomous solution leading to a paradigm change by designing a fully integrated all-optical wireless monolithic photoelectrochemical device based on a nanostructured Si photovoltaic junction modified with catalytic coatings. Under illumination with light ranging from visible to near-infrared, photogenerated holes induce the oxidation of the ECL reagents and thus the emission of visible ECL photons. The blue ECL emission is easily viewed with naked eyes and recorded with a smartphone. A new light emission scheme is thus introduced where the ECL emission energy (2.82 eV) is higher than the excitation energy (1.18 eV) via an intermediate electrochemical process. In addition, the mapping of the photoelectrochemical activity by optical microscopy reveals the minority carrier interfacial transfer mechanism at the nanoscale. This breakthrough provides an all-optical strategy for generalizing ECL without the need for electrochemical setups, electrodes, wiring constraints, and specific electrochemical knowledge. This simplest ECL configuration reported so far opens new opportunities to develop imaging and wireless bioanalytical systems such as portable point-of-care sensing devices.

更新日期：2023-07-27

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