College of Chemistry and Pharmaceutical Sciences, Qingdao Agricultural University, Qingdao 266109, P. R. China.
Anal Chem. 2021 Sep 14;93(36):12441-12446. doi: 10.1021/acs.analchem.1c02605. Epub 2021 Aug 31.
The classic luminol-based electrochemiluminescence (ECL) platform generally suffers from self-decomposition of the coreactant (i.e., HO) during the reaction process, seriously hampering the luminous signal stability, as well as its practical application. To address this issue, apart from the introduction of complex exogenous species, preoxidation of the luminophore, and electrocatalysis for ECL signal amplification, we proposed a novel ECL model to realize the signal enhancement via self-photocatalytic generation of the coreactant HO. Interestingly, the luminescence of luminol was simultaneously utilized as the light source to promote the conversation of O to HO with the assistance of the photocatalyst resorcinol-formaldehyde resin, which could further improve the luminescence of luminol in turn. In comparison with the traditional case, this new ECL model not only exhibited obvious signal amplification but also efficiently boosted its stability of signal output. To sum up, an exogenous coreactant-free, highly stable ECL platform was obtained via simply integrating the photocatalyst RF and the luminol-based system. This work will not only inspire the design of a new integrated ECL system with a coreactant translator but also provide an ingenious insight for the construction of a new generation of ECL models.
基于鲁米诺的经典电化学发光（ECL）平台通常在反应过程中会遭受核心反应物（即 HO）的自分解，这严重阻碍了发光信号的稳定性及其实际应用。为了解决这个问题，除了引入复杂的外源性物质、预氧化发光体和电催化放大 ECL 信号外，我们还提出了一种新的 ECL 模型，通过核心反应物 HO 的自光催化生成来实现信号增强。有趣的是，鲁米诺的发光同时被用作光源，在光催化剂间苯二酚-甲醛树脂的协助下促进 O 到 HO 的转化，这反过来又可以进一步提高鲁米诺的发光。与传统情况相比，这种新的 ECL 模型不仅表现出明显的信号放大，而且还有效地提高了信号输出的稳定性。总之，通过简单地集成光催化剂 RF 和基于鲁米诺的系统，获得了一种无需外加核心反应物、高度稳定的 ECL 平台。这项工作不仅将激发具有核心反应物转化器的新型集成 ECL 系统的设计，而且还为新一代 ECL 模型的构建提供了巧妙的见解。
