Rational Design of a Highly Dispersed Fe–N–C Nanosheet with 1,10-Phenanthroline-2,9-Dicarboxylic Acid as a Preorganized Ligand: Boosted Electrochemiluminescence Detection of Tetracycline,Analytical Chemistry

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Rational Design of a Highly Dispersed Fe–N–C Nanosheet with 1,10-Phenanthroline-2,9-Dicarboxylic Acid as a Preorganized Ligand: Boosted Electrochemiluminescence Detection of Tetracycline
Analytical Chemistry ( IF 6.7 ) Pub Date : 2021-12-23 , DOI: 10.1021/acs.analchem.1c04558
Li-Ping Zong ₁ , Junji Li ₁ , Guofang Shu ₂ , Xinye Liu _{1,

3} , Robert S Marks ₄ , Xue-Ji Zhang _{1,

5} , Serge Cosnier ₆ , Dan Shan ₁

Affiliation

In view of the shortcomings of the current coreactant electrochemiluminescence (ECL) and inspired by natural oxygen (O₂) reduction metalloenzymes, a novel ECL amplification strategy was established. A pyrolytic iron- and nitrogen-doped (Fe–N–C) nanosheet rich in singly ionized oxygen vacancy (V_O^•) defects was rationally designed by destroying the highly saturated coordination with a preorganized ligand 1,10-phenanthroline-2,9-dicarboxylic acid (PDA). Extraordinary catalytic activity for O₂ activation was obtained via screening a special pyrolysis temperature using spectroscopic and electrochemical methods. The high-spin ferric centers of highly dispersed FeC nanoclusters and 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 O₂ and simultaneously shorten the transferring distance of radicals. Tetracycline (TC), which posed a growing threat to aquatic biodiversity and environmental safety, as a 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.

中文翻译：

以 1,10-菲咯啉-2,9-二羧酸为预组织配体的高分散 Fe-N-C 纳米片的合理设计：四环素的增强电化学发光检测

针对目前共反应物电化学发光（ECL）的不足，并受天然氧（O ₂）还原金属酶的启发，建立了一种新型的ECL放大策略。通过破坏与预组织配体 1,10-phenanthroline-2,9 的高度饱和配位，合理设计了富含单电离氧空位 (V _O^• ) 缺陷的热解铁和氮掺杂 (Fe-N-C) 纳米片-二羧酸（PDA）。_{对 O 2}具有非凡的催化活性通过使用光谱和电化学方法筛选特殊的热解温度来获得活化。高度分散的 Fe3C 纳米团簇的高自旋铁中心和丰富的碳和氧空位缺陷充分促进了固有的催化活性。ECL 放大是通过将材料与鲁米诺整合以从溶解的 O ₂原位产生氧化还原活性自由基来实现的同时缩短自由基的转移距离。对水生生物多样性和环境安全构成日益严重威胁的四环素（TC）作为一种模式抗生素被成功检测到，检测限为3.88 nM（S/N = 3），阐明了这种新型有效ECL扩增的广阔应用前景生物分析和环境监测策略。

更新日期：2022-01-18

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