It is vital to monitor the level of biological species, especially antioxidants including ascorbic acid (AA) and other biothiols related to human health. Conventional methods usually relied on target-specific sensing strategy and lacked discrimination of targets with similar structures. In this work, we introduced a novel dual lanthanide-doped nanoprobe (Ce/Tb-ATP) and constructed the sensor array according to luminescent signals. In the presence of ATP, Ce3+ could emit its specific luminescence and sensitize Tb3+ through an energy transfer process, which provided a dual-signal mode (Ce: 350 nm, Tb: 546 nm) under UV excitation. Chemical active Ce3+ was popular in many redox reactions with valence state changes between +3 and +4. By combination of H2O2, Ce/Tb-ATP nanoprobe was disassembled and the dual-signal luminescence intensity would quench. However, human-related antioxidants, AA, cysteine (Cys), homocysteine (Hcys) and glutathione (GSH) could also efficiently react with H2O2, which prohibited the oxidation of Ce3+ and luminescence would recover to different extents. Through density functional theory (DFT) calculations, these antioxidants had variety in reduction potentials and supported the novel principal component analysis (PCA) of each by using luminescence signals as basic elements. In view of similar biochemical mechanism in living body, H2O2 generated from glucose/glucose oxidase (Glu/GOx) reaction was also promoted to realize the novel bioassays. Two formats of chemical sensor array based on Ce/Tb-ATP nanoprobe were achieved by regulation of a series of redox reactions. This work emphasized the potential applications of Ce/Tb-ATP nanoprobe in discrimination of antioxidants and was expected to be well applied in the early diagnosis of diseases caused by the abnormal content of antioxidants.

Design of cerium/terbium-based nanoprobe and applications in antioxidants discrimination analysis

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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