A self-calibrating logic system and oxidase-based biosensor using Tb3+-doped carbon dots/DNA conjugates

Tb 3+ -doped carbon dots (Tb 3+ @CDs) were prepared in a facile hydrothermal method by using ammonium citrate as carbon source and Tb 3+ as dopant. A 15-bp GT-rich single-strand DNA (ssDNA) was introduced to sensitize Tb 3+ via the antenna effect for generating two fluorescence signals (CDs and Tb 3+ ), forming a conjugate of Tb 3+ @CDs/ssDNA. The ratiometric fluorescence of Tb 3+ @CDs/ssDNA could be reversibly regulated by Ag + and Cys, in which the fluorescence peak at 546 nm of Tb 3+ could be switched to “On” or “Off” as the signal indicator while the fluorescence peak at 444 nm of CDs remained constant as the build-in reference. The proposed Ag + /Cys-mediated reversible fluorescence changes in Tb 3+ @CDs/ssDNA was also proven for the design of a self-calibrating ratiometric fluorescence logic system. By integrated with the specific reaction between H 2 O 2 and Cys, Tb 3+ @CDs/ssDNA was applied for ratiometric fluorescence detection of H 2 O 2 . More importantly, the sensing strategy could be further successfully extended to the monitoring of H 2 O 2 -produced oxidase-related reactions, such as GOx-biocatalyzed oxidation of glucose (the limit of detection: 0.06 μM) and was well applied in rat serum compared to commercial kits. This work unveiled a novel ratiometric fluorescent design, which is cost-effective, simple to prepare and easy-to-use without chemical modification or fluorescence labeling .