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The concept of a lab-on-a-molecule, which was proposed just short of two decades ago, has captured the imagination of scientists. From originally being proposed as an AND logic gate driven by three chemical inputs as a direct way of detecting congregations of chemical species, the definition of what constitutes a lab-on-a-molecule has broadened over the years. In this review, molecules that can detect multiple analytes by fluorescence, among other techniques, are reviewed and discussed, in the context of molecular logic and multi-analyte sensing. The review highlights challenges and suggestions for moving the frontiers of research in this field to the next dimension.

H2O and D2O are an important pair of analogues, and their high-efficient detections are closely related to fields of chemical industry, food processing, semiconductor, environmental monitoring, etc. Because of their extremely similar physical and chemical properties, H2O and D2O can be mutually soluble in any ratios, and it is generally thought that the discrimination of H2O and D2O is an enormous challenge. Herein, upon the fact that vibrational frequency of O-H is greater than O-D, we design a dynamic Eu(III)-macrocycle Eu-2a with two emitters which exhibits the imine bond breakage of macrocycle emitter H2L2a in H2O or D2O, resulting in the turn-on fluorescence of Eu(III) emitter. For their differential fluorescence sensing signals of Eu-2a on three emission bands (433, 500 and 615 nm), the statistical analysis method is employed to produce fully separated fingerprints and thus high-throughput discrimination of 13 common solvents, especially the H2O and D2O. Fluorescent titration experiments by instrumental or smartphone-based analysis method also prove the successful determination of proportional H2O/D2O mixtures together with the good sensitivity and wide linear response range. Moreover, this H2O-triggered fluorescent complex Eu-2a used as the fluorescence ink also shows its potential in information encryption application. This article must be a valuable reference for the areas of lanthanide-based luminescent material, multianalyte detection and information encryption.

Multianalyte detection and analogue discrimination are extremely valuable frontier areas for their wide applications in environmental, medical, clinical and industrial analyses. Nowadays, researchers rack their brains on how to develop excellent multianalyte chemosensors that have presented huge challenges in designing high-efficient fluorescent sensing materials and constructing high-throughput detection methods. In this paper, we propose a novel strategy to utilize the dual-emission fluorescent detection platform as a lab-on-a-molecule, arising from the disalicylaldehyde-coordinated hybrid H2Qj3/Tb based terbium sensibilization coupled excited-state intramolecular proton transfer effects. Using the statistical analysis (PCA and HCA) for sensing signals of three fluorescence channels (431, 543 and 583 nm), we demonstrate this elaborate chemosensor with multianalyte detection of three species (solvents, anions and cations) and pattern discrimination of analogues. As a result, the H2Qj3/Tb shows great lab-on-a-molecule characters for each set of species, resulting in the easier identification of many critical analytes (e.g., H2O, NO2- and Fe3+) and discrimination of analogues. In addition, it is also proven to be able to provide reliable content determination for an analyte, especially the NO2- (LOD = 0.37 μM), and discrimination for mixed analogues. A combination of easy-to-implement preparation procedure and data analysis technique makes this work promising for not only designing similar lanthanide-based materials but also realizing more high-efficient multianalyte sensing systems towards various potential applications.

A polymer chemical sensor based on lab-on-a-molecule was synthesised by amine-aldehyde polymerisation for selective detection of fluorine ions (F-) and cyanide (CN-). The polymer chemical sensor shows significant absorption and fluorescence changes upon the addition of F- and CN-, which can be observed by the naked eye and optical reactions. The polymer has a higher fluorescence enhancement effect than its monomer and the distance of wavelength of each anion increased which could be applied to better distinguish the two anions.