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Robust Fluorescent Eutectogel with Temperature Resilience and Microenvironment-Regulated Emission for
Huanhuan Dong1, Xinyu Gou1, Nianhua Zhao1
1Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education Shaanxi Provincial Key Laboratory of New Concept Sensors and Molecular Materials, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an710119, P. R. China.
Abstract:
Fluorescent eutectogels, as emerging smart materials that integrate the unique microenvironment, excellent temperature resistance, and eco-friendliness of deep eutectic solvents (DESs), have driven remarkable advancement in flexible optical materials and information encryption. Here we report a transparent fluorescent eutectogel prepared by incorporating the environmentally sensitive cationic luminophore 2,5-bis(2-pyridiniumyl)-1H-pyrrole bis(hexafluorophosphate) ([H3DPP]2+) into a glycerol/Zn(NO3)2·6H2O DES followed by in situ photopolymerization of acrylamide. The nitrate-containing DES strongly reshapes the photophysical behavior of [H3DPP]2+, producing a pronounced red shift and enhanced emission relative to glycerol or aqueous Zn(NO3)2 solution. The addition of monomer has little influence on the DES-regulated emission, whereas gel-network formation causes only moderate fluorescence attenuation while largely preserving the DES-defined emissive state. Spectroscopic analysis and DFT/TD-DFT calculations indicate that directional hydrogen-bonding interactions between NO3- and the protonated/pyrrolic N-H sites of [H3DPP]2+ modulate its electronic structure and optical transitions. The resulting eutectogel exhibits high visible transparency, tensile strength of 230 kPa, stretchability of 820%, adhesion to diverse substrates (0.25 MPa on PTFE), and excellent solvent retention, maintaining 95% of its solvent after storage at 70 °C for 9 days. The fluorescence also remains visible after prolonged storage at 25, 70, and -25 °C. Moreover, relying on the high transparency, good mechanical properties and stimulus-responsive fluorescence characteristics of this eutectogel, localized chemical writing, UV-triggered visualization and barcode digital reading can be realized. This work demonstrates that DES-regulated microenvironments offer a robust platform for tuning molecular emission and developing stable, stimuli-responsive fluorescent soft materials for visual anticounterfeiting and information encryption.
