华中师范大学Chengzhou Zhu研究小组报道了，在NiIr单原子合金气凝胶上调整电化学水活化以实现稳定的电化学发光(ECL)。2024年4月22日出版的《科学通报》杂志发表了这项成果。

阳极析氧反应是传统水基ECL系统中公认的副反应，由于氧在电极处的生成和表面聚集，对ECL发光的稳定性和效率产生不利影响。然而，水氧化过程中产生的活性氧对ECL发光团的影响在很大程度上被忽视了。以典型的鲁米诺发射器为例，在该研究中，团队采用具有高效水氧化活性的NiIr单原子合金气凝胶作为原型共反应促进剂，首次阐明了ECL行为与水氧化反应动力学之间的关系。

团队通过调节电解液中氢氧化物离子的浓度，对鲁米诺和水的电化学氧化过程进行了微调。当电解质中氢氧离子浓度较低时，水的氧化动力学减弱，这限制了氧的产生，有效地减轻了氧积累对ECL强度的影响，为ECL系统中副反应的处理提供了新的视角。最后，团队构建了一种灵敏、稳定的抗氧化检测传感器，并将其应用于实际样品检测中。

附：英文原文

Title: Tuning electrochemical water activation over NiIr single-atom alloy aerogels for stable electrochemiluminescence

Author: Liuyong Hu b, Wenling Gu a, Chengzhou Zhu a

Issue&Volume: 2024/04/22

Abstract: The anodic oxygen evolution reaction is a well-acknowledged side reaction in traditional aqueous electrochemiluminescence (ECL) systems due to the generation and surface aggregation of oxygen at the electrode, which detrimentally impacts the stability and efficiency of ECL emission. However, the effect of reactive oxygen species generated during water oxidation on ECL luminophores has been largely overlooked. Taking the typical luminol emitter as an example, herein, we employed NiIr single-atom alloy aerogels possessing efficient water oxidation activity as a prototype co-reaction accelerator to elucidate the relationship between ECL behavior and water oxidation reaction kinetics for the first time. By regulating the concentration of hydroxide ions in the electrolyte, the electrochemical oxidation processes of both luminol and water are finely tuned. When the concentration of hydroxide ions in electrolyte is low, the kinetics of water oxidation is attenuated, which limits the generation of oxygen, effectively mitigates the influence of oxygen accumulation on the ECL strength, and offers a novel perspective for harnessing side reactions in ECL systems. Finally, a sensitive and stable sensor for antioxidant detection was constructed and applied to the practical sample detection.

DOI: 10.1016/j.scib.2024.04.038

Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927324002792