RESUMO
The fabrication of an all-in-one solid-state ECL sensing platform is beneficial not only for expediting the miniaturization of sensing devices, but also, more importantly, for enabling point-of-care applications. In the present work, a self-enhanced solid-state ECL sensing platform is fabricated using newly synthesised silica polyethylene nanoparticles (SiO2-PEI NPs) which generate a co-reactant in situ and easily self-assemble with Ru(bpy)32+ and shows selective and sensitive detection of spermine at physiological pH (7.4). Spermine induces the maximum ECL emission intensity compared to other biogenic amines due to the presence of two secondary amines. A possible ECL reaction mechanism has been proposed based on CV and ECL experiments, DFT calculations, and in situ ECL spectrum analysis. The developed solid-state sensor showed a linear increase in ECL intensity with increasing spermine concentration in the range of 10 nM to 100 nM with an LOD of 12.2 nM. Compared to other biogenic amines in previous works, chemically synthesised SiO2-PEI NPs used in the present study act as an effective label- and enzyme-free sensor, and the new method is observed to be simple and cost-effective, to overcome various limitations of solution-phase ECL and to avoid the usage of any noble metals.
RESUMO
In recent years, electrochemiluminescence (ECL) has received enormous attention and has emerged as one of the most successful tools in the field of analytical science. Compared with homogeneous ECL, the heterogeneous (or solid-state) ECL has enhanced the rate of the electron transfer kinetics and offers rapid response time, which is highly beneficial in point-of-care and clinical applications. In ECL, the luminophore is the key element, which dictates the overall performance of the ECL-based sensors in various analytical applications. Tris(2,2'-bipyridyl)ruthenium (II) complex, Ru(bpy)32+, is a coordination compound, which is the gold-standard luminophore in ECL. It has played a key role in translating ECL from a "laboratory curiosity" to a commercial analytical instrument for diagnosis. The aim of the present review is to provide the principles of ECL and classical reaction mechanisms-particularly involving the heterogeneous Ru(bpy)32+/co-reactant ECL systems, as well as the fabrication methods and its importance over solution-phase Ru(bpy)32+ ECL. Then, we discussed the emerging technology in solid-state Ru(bpy)32+ ECL-sensing platforms and their recent potential analytical applications such as in immunoassay sensors, DNA sensors, aptasensors, bio-imaging, latent fingerprint detection, point-of-care testing, and detection of non-biomolecules. Finally, we also briefly cover the recent advances in solid-state Ru(bpy)32+ ECL coupled with the hyphenated techniques.
RESUMO
Correction for 'Study of highly stable electrochemiluminescence from [Ru(bpy)3]2+/dicyclohexylamine and its application in visualizing sebaceous fingerprint' by Mathavan Sornambigai et al., Chem. Commun., 2022, 58, 7305-7308, https://doi.org/10.1039/D2CC01929A.
RESUMO
For the first time, we report a novel and highly stable visual electrochemiluminescence emission from the [Ru(bpy)3]2+/dicyclohexylamine system at physiological pH conditions, with a quantum efficiency (ΦECL) of 95.5%. Furthermore, we have successfully demonstrated the simple and rapid smartphone-based ECL mapping of sebaceous fingerprints via a non-destructive mode.
Assuntos
Medições Luminescentes , CicloexilaminasRESUMO
Though luminol is one of the most prominent and extensively studied luminophores in ECL studies, only H2O2 has been widely used as a co-reactant. This limits the variety of applications because of the short-time radical stability and low quantum efficiency. In the present work, we identified dicyclohexylamine (DCHA) as a new and highly efficient anodic co-reactant in ECL for the luminol molecule. The electrochemical and ECL behavior of the luminol/DCHA system was studied on a simple bare GCE surface, which results in two anodic ECL peaks at the potential region of +0.38 and +0.94 V vs Ag/AgCl. The evidence of (DCHAâ¢+) and O2â¢- generated in the system was detected via flat-cell electron spin resonance (ESR) spectroscopy experiments at â¼20 °C. Using the bimodal ECL system, the highly sensitive detection of luminol was achieved with the detection limit down to 1.5 pM. Further, a homebuilt electrochemiluminescent detector coupled with a flow injection analysis (ECL-FIA) system was adopted to detect the DCHA contaminant in harvested honey, which achieved higher detection and sensitivity under the optimized experimental conditions. DCHA was detected in the range of 10 nM to 100 µM with the detection limit of 2 nM (S/N = 3). The present findings of new luminol/DCHA ECL signals produced a strong ECL emission, which leads to a greater potential to meet the fast-developing analytical application of a luminol-based ECL system.
