Single‐Atom Iron Boosts Electrochemiluminescence

Abstract

The traditional luminol–H2O2 electrochemiluminescence (ECL) sensing platform suffers from self‐decomposition of H2O2 at room temperature, hampering its application for quantitative analysis. In this work, for the first time we employ iron single‐atom catalysts (Fe‐N‐C SACs) as an advanced co‐reactant accelerator to directly reduce the dissolved oxygen (O2) to reactive oxygen species (ROS). Owing to the unique electronic structure and catalytic activity of Fe‐N‐C SACs, large amounts of ROS are efficiently produced, which then react with the luminol anion radical and significantly amplify the luminol ECL emission. Under the optimum conditions, a Fe‐N‐C SACs–luminol ECL sensor for antioxidant capacity measurement was developed with a good linear range from 0.8 μm to 1.0 mm of Trolox.

Iron-based single-atom electrocatalysts: synthetic strategies and applications

“…9). Gu et al 36 mixed glucose, dicyandiamide, and ferrous chloride tetrahydrate in an aqueous solution and then carried out freeze-drying and pyrolysis to obtain monoatomic catalyst Fe-N-C. Serov et al 23 prepared monoatomic catalyst Fe-CBDZ by pyrolysis and acid etching using ferric nitrate and carbendazim as precursors and SiO 2 powder as a template. Owing to the elimination of articial carbon in the material design, the unique process method, and the reasonable selection of precursors based on high carbon content, high N/C ratio and low volatile content, the catalyst showed a higher active site density and a higher mass activity.…”

Electroactive Metal–Organic Frameworks as Emitters for Self‐Enhanced Electrochemiluminescence in Aqueous Medium

“…Typically, pre‐oxidation of methionine‐stabilized gold nanoclusters resulted in a 66 % anodic ECL yield . The iron single‐atom catalysts reduced the dissolved oxygen into reactive oxygen species to increase the ECL signal in luminol–O 2 system . Herein, a self‐enhanced strategy is developed based on radical accumulation of electroactive MOF (E‐MOF) as emitter in aqueous medium.…”

“…[16] To amplify the signal for readout, a series of amplification strategies were developed through intramolecular electron transfer, [17] pre-oxidation, [18] and electrocatalysis, and so on. [19] Typically, pre-oxidation of methionine-stabilized gold nanoclusters resulted in a 66 % anodic ECL yield. [18] The iron single-atom catalysts reduced the dissolved oxygen into reactive oxygen species to increase the ECL signal in luminol-O 2 system.…”

Fluorescent Noble Metal Nanoclusters Loaded Protein Hydrogel Exhibiting Anti‐Biofouling and Self‐Healing Properties for Electrochemiluminescence Biosensing Applications

“…[ 1–3 ] By far, remarkable efforts have been made to develop various types of ECL based biosensing systems, [ 4,5 ] and the recent introduction of new ECL materials or mechanisms, such as metal‐organic frameworks, aggregation‐induced emission luminogens or single atom catalysts, further improved the performance and application ranges of ECL based biosensing systems. [ 6–11 ] However, as a method extremely sensitive to the state of the electrode surface, nonspecific adsorption of biological macromolecules, in particular proteins, and physical scratches of the electrode surfaces, during the sensing of complex biological samples, severely affects the accuracy and practical applicability of the ECL biosensing systems. [ 12 ] In order to meet the requirements of anti‐interference and long‐term application in practical biosensing applications, it is highly demanded to develop ECL biosensing systems with anti‐biofouling and self‐healing properties.…”