期刊
ANALYTICAL CHEMISTRY
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.2c01794
关键词
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资金
- National Natural Science Foundation of China [22004042, 22074049, 22104144]
- Natural Science Foundation of Hubei Province [2020CFB276, 2021CFB518]
- Open Funds of the State Key Laboratory of Electroanalytical Chemistry [SKLEAC202102]
- self-determined research funds of the CCNU from the colleges' basic research and operation of MOE [CCNU20QN007, CCNU20TS013]
- Program of Introducing Talents of Discipline to Universities of China (111 program) [B17019]
- Beijing Synchrotron Radiation Facility
In this study, iron single-atom catalysts were used as efficient co-reaction accelerators to achieve strong cathodic electrochemiluminescence at an ultralow potential. The catalysts activate H2O2 to produce reactive oxygen species, which directly react with a luminol to generate intense emission.
The conventional cathodic electrochemiluminescence (ECL) always requires a more negative potential to trigger strong emission, which inevitably damages the bioactivity of targets and decreases the sensitivity and specificity. In this work, iron single-atom catalysts (Fe-N-C SACs) were employed as an efficient co-reaction accelerator for the first time to achieve the impressively cathodic emission of a luminol-H2O2 ECL system at an ultralow potential. Benefiting from the distinct electronic structure, Fe-N-C SACs exhibit remarkable properties for the activation of H2O2 to produce massive reactive oxygen species (ROS) under a negative scanning potential from 0 to -0.2 V. The ROS can oxidize the luminol anions into luminol anion radicals, avoiding the tedious electrochemical oxidation process of luminol. Then, the in situ-formed luminol anion radicals will directly react with ROS for the strong ECL emission. As a proof of concept, sensitive detection of the carcinoembryonic antigen was realized by glucose oxidase-mediated ECL immunoassay, shedding light on the superiority of SACs to construct efficient cathodic ECL systems with low triggering potential.
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