Microdroplet-Mediated Radical Polymerization.

Micrometer-sized aqueous droplets serve as a unique reactor that drives various chemical reactions not seen in bulk solutions. However, their utilization has been limited to the synthesis of low molecular weight products at low reactant concentrations (nM to µM). Moreover, the nature of chemical reactions occurring outside the droplet remains unknown. This study demonstrated that oil-confined aqueous microdroplets continuously generated hydroxyl radicals near the interface and enabled the synthesis of polymers at high reactant concentrations (mM to M), thus successfully converting the interfacial energy into the synthesis of polymeric materials. The polymerized products maintained the properties of controlled radical polymerization, and a triblock copolymer with tapered interfaces was prepared by the sequential addition of different monomers into the aqueous microdroplets. Furthermore, a polymerization reaction in the continuous oil phase was effectively achieved by the transport of the hydroxyl radicals through the oil/water interface. This interfacial phenomenon is also successfully applied to the chain extension of a hydrophilic polymer with an oil-soluble monomer across the microdroplet interface. Our comprehensive study of radical polymerization using compartmentalization in microdroplets is expected to have important implications for the emerging field of microdroplet chemistry and polymerization in cellular biochemistry without any invasive chemical initiators.

In Situ Supramolecular Polymerization of Micellar Nanoobjects Induced by Polymerization.

Supramolecular polymerization offers a fascinating opportunity to develop dynamic soft materials by associating monomeric building blocks via noncovalent interactions. We report that polymerization can spontaneously drive the supramolecular polymerization of nanoscale micellar objects. We constructed the patchy micelles via two-step polymerization-induced self-assembly. A horizontal association between the patches results in a 1D supermicellar chain in situ by minimizing the enthalpic penalty of exposing the growing chains to solvent. Its length grows with increasing degree of polymerization, confirming that the supramolecular polymerization was triggered and controlled by polymerization. Our results highlight the observation that (1) the entire self-assembly process of forming, compartmentalizing, and associating the micelles can be driven by polymerization in a concerted manner and that (2) polymerization-induced self-assembly now can use compartmentalized nanoobjects as substrates beyond block copolymer chains. Polymerization-induced supramolecular polymerization could be useful for the autonomous preparation of hierarchical nanostructures.

Green Synthesis of Laser-Induced Graphene with Copper Oxide Nanoparticles for Deicing Based on Photo-Electrothermal Effect.

Homogenously dispersed Cu oxide nanoparticles on laser-induced graphene (LIG) were fabricated using a simple two-step laser irradiation. This work emphasized the synergetic photo-electrothermal effect in Cu oxide particles embedded in LIG. Our flexible hybrid composites exhibited high mechanical durability and excellent thermal properties. Moreover, the Cu oxide nanoparticles in the carbon matrix of LIG enhanced the light trapping and multiple electron internal scattering for the electrothermal effect. The best conditions for deicing devices were also studied by controlling the amount of Cu solution. The deicing performance of the sample was demonstrated, and the results indicate that the developed method could be a promising strategy for maintaining lightness, efficiency, excellent thermal performance, and eco-friendly 3D processing capabilities.

Laser-Induced Graphene Heater Pad for De-Icing.

The replacement of electro-thermal material in heaters with lighter and easy-to-process materials has been extensively studied. In this study, we demonstrate that laser-induced graphene (LIG) patterns could be a good candidate for the electro-thermal pad. We fabricated LIG heaters with various thermal patterns on the commercial polyimide films according to laser scanning speed using an ultraviolet pulsed laser. We adopted laser direct writing (LDW) to irradiate on the substrates with computer-aided 2D CAD circuit data under ambient conditions. Our highly conductive and flexible heater was investigated by scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, X-ray diffraction, and Brunauer-Emmett-Teller. The influence of laser scanning speed was evaluated for electrical properties, thermal performance, and durability. Our LIG heater showed promising characteristics such as high porosity, light weight, and small thickness. Furthermore, they demonstrated a rapid response time, reaching equilibrium in less than 3 s, and achieved temperatures up to 190 °C using relatively low DC voltages of approximately 10 V. Our LIG heater can be utilized for human wearable thermal pads and ice protection for industrial applications.

Highly Skin-Conformal Laser-Induced Graphene-Based Human Motion Monitoring Sensor.

Bio-compatible strain sensors based on elastomeric conductive polymer composites play pivotal roles in human monitoring devices. However, fabricating highly sensitive and skin-like (flexible and stretchable) strain sensors with broad working range is still an enormous challenge. Herein, we report on a novel fabrication technology for building elastomeric conductive skin-like composite by mixing polymer solutions. Our e-skin substrates were fabricated according to the weight of polydimethylsiloxane (PDMS) and photosensitive polyimide (PSPI) solutions, which could control substrate color. An e-skin and 3-D flexible strain sensor was developed with the formation of laser induced graphene (LIG) on the skin-like substrates. For a one-step process, Laser direct writing (LDW) was employed to construct superior durable LIG/PDMS/PSPI composites with a closed-pore porous structure. Graphene sheets of LIG coated on the closed-porous structure constitute a deformable conductive path. The LIG integrated with the closed-porous structure intensifies the deformation of the conductive network when tensile strain is applied, which enhances the sensitivity. Our sensor can efficiently monitor not only energetic human motions but also subtle oscillation and physiological signals for intelligent sound sensing. The skin-like strain sensor showed a perfect combination of ultrawide sensing range (120% strain), large sensitivity (gauge factor of ~380), short response time (90 ms) and recovery time (140 ms), as well as superior stability. Our sensor has great potential for innovative applications in wearable health-monitoring devices, robot tactile systems, and human-machine interface systems.