One-step Fabrication of Physical Eutectogel with Recyclability: Crystalline Domain Regulation Induced by Microgels.

HYPOTHESIS: Despite their non-volatility, low cost, and recyclability, physical eutectogels' appeal is hindered by the intricate fabrication process and the involvement of hazardous chemicals. The network of polyvinyl alcohol (PVA) in deep eutectic solvent (choline chloride and glycerol) might be developed by the addition of microgels of polyacrylic acid (Carbopol). EXPERIMENTS: Hydrogen-bond interactions between Carbopol and PVA are revealed through Fourier-transform infrared spectroscopy. The impact of microgels on crystalline domains and the polymer network can be observed using X-ray diffraction and scanning electron microscopy. The physical properties of the eutectogel, including mechanical strength and ionic conductivity, are investigated as well. Finally, the strain-sensing ability and remarkable recyclability of the eutectogel are demonstrated. FINDINGS: The physical eutectogel can be obtained through a one-step fabrication process using only green and low-cost materials. It demonstrates robust strength (1.02 MPa) and remarkable stretchability (1000 % strain). This is attributed to the uniform dispersion of PVA crystalline domains within the deep eutectic solvent, facilitated by the hydrogen bonds and space restriction effects between PVA and Carbopol. Furthermore, the physical eutectogel with recyclability can consistently generate electrical resistance signals, highlighting its potential as a reliable strain sensor.

Jammed Microgels in Deep Eutectic Solvents as a Green and Low-Cost Ink for 3D Printing of Reliable Auxetic Strain Sensors.

Additive manufacturing is a promising technique for offering novel functionality to various materials by creating three-dimensional (3D) structures. However, the development of sustainable synthesis processes for 3D printing inks or 3D-printed materials remains a major challenge. In this work, a simple two-step mixing approach is developed to prepare a 3D printing ink from green, low-cost, and low-toxicity materials [commercial Carbopol and deep eutectic solvents (DESs)]. A small weight fraction of Carbopol can impart desired rheological properties to the DES used in the 3D printing ink and also can significantly enhance the stretchability of eutectogels up to 2500% strain. The 3D-printed auxetic structure shows a negative Poisson's ratio (within 100% strain), high stretchability (300%), high sensitivity (gauge factor of 3.1), good moisture resistance, and sufficient transparency. It can detect human motion with high skin comfort and breathability. The results of this work highlight a green, low-cost, and energy-saving strategy to fabricate conductive microgel-based inks for 3D printing of wearable devices.