Rational design of highly dispersed Fe-N-C based on 1,10phenanthroline-2,9-dicarboxylic acid as preorganized ligand for precursor: boosted electrochemiluminescence detection of tetracycline
Résumé
In view of the shortcomings of the current coreactant electrochemiluminescence (ECL) and inspired by natural oxygen (O 2) reduction metalloenzymes, a novel ECL amplification strategy was established. A pyrolytic iron and nitrogen-doped (Fe-N-C) material rich in V O • defects was rationally designed by destroying the highly saturated coordination with preorganized ligand PDA. Extraordinary catalytic activity for O 2 activation was obtained via screening a special pyrolysis temperature using spectroscopic and electrochemical methods. The high-spin ferric centers of highly dispersed FeC nanoclusters, abundant carbon and oxygen vacancy defects, fully contributed to the inherent catalytic activity. ECL amplification was achieved by integrating the material with luminol to generate redox active radicals in situ from dissolved O 2 and simultaneously shorten the transferring distance of radicals. Tetracycline (TC), which posed a growing threat to aquatic biodiversity and environmental safety, as the model antibiotic was successfully detected with a detection limit of 3.88 nM (S/N = 3), clarifying a promising application prospect of this new effective ECL amplification strategy in biological analysis and environmental monitoring.
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