Programmable-Printing Paper-Based Device with a MoS2 NP and Gmp/Eu-Cit Fluorescence Couple for Ratiometric Tetracycline Analysis in Various Natural Samples

Paper-based fluorescence devices, with smartphone aids, bring considerable operation convenience for tetracycline (TC) sensing. Nevertheless, they must meet the challenge in real determination against complicated backgrounds. Considering that, we present a programmable-printing paper-based device and then apply it to TC determination for various natural samples. MoS2 NPs and Gmp/Eu-Cit are synthetized as composite probes. A static quenching process is found with MoS2 NP fluorescence at 430 nm, while significant magnification of Gmp/Eu-Cit emission is obtained at 617 nm, establishing a valuable ratiometric indicator. Remarkably, two-stage programmable printing maximizes the proposed sensing capability. A transitive device, containing a gradually changing amount of a certain probe, is prepared to sense TC. With a homemade smartphone application and 3D-printed measurement chamber, the corresponding signals are examined to explore optimal setups. These setups are automatically processed to prepare the final-version device, not requiring manual operations. Benefitting from this interesting feature, the proposed device gains many rewards in performances. It effectively senses TC in a wide range from 12.7 nM to 80 μM and simultaneously provides naked eye-legible signals and smartphone-based readouts with confident selectivity and stability. This device is consequently applied for various samples of soil, river water, milk, and serum and meets well with HPLC-MS and recovery tests.