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Schematic illustrating synthesis of millimeter-sized hydrophobic polypyrrole-coated polystyrene (PS/PPy-C8F) particles by aqueous chemical oxidative seeded polymerization and fabrication of near-spherical liquid marble (LM), followed by shape designing toward non-spherical LM.
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... this communication, there are two objectives (Figure 1): (i) Synthesis of near-monodispersed 'millimeter'-sized polymer particles coated by a hydrophobic polymer overlayer by seeded polymerization. The seeded polymerization is one of powerful methods to design/modify surface chemistry of the particles 18-21 . ...
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... polystyrene (PS) particles coated by hydrophobic polypyrrole (PPy) overlayer doped with perfluoroalkyl dopant (PS/PPy-C8F particles) were synthesized by aqueous chemical oxidative seeded polymerization of pyrrole (Py) with heptadecafluorooctanesulfonic acid (C8F) as a hydrophobic dopant in the presence of 1 mm-sized PS seed particles 24,30 ( Figure S1). Py monomer (10 mg) was added to an aqueous dispersion of the PS seed particles (12 g PS particles in 70 g water, the volume-average diameter (Dv) in water, 1027 ± 250 µm; the number-average particle diameter (Dn), 1044 ± 26 µm) and left to stirring for 3 h. ...
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Citations
... Other than the sol-gel technique, hexagonal fluorinated poly(ethylene terephthalate) (PET) plates, silica powder, polystyrene particles, and steric acid powder have also been reported for accurate shaping of LM [118,[138][139][140]. Bormashenko et al reported the first-ever shaped LM [141]. ...
Particle-coated liquid entities are the basis of many useful products, such as foams, emulsions, bijels, and liquid marbles. Particles stabilized at the liquid-air interface have been widely explored during the past two decades. Such interfaces usually consist of micro- to nano-sized particles that often tend to aggregate and lose transparency as well as the smoothness of the interface. Recently, these obstacles have been overcome by using sol-gel-derived silica nanoparticle coating. Sol-gel-derived nanoparticles offer a monolayer structure at the interface with high transparency and reproducibility. This paper critically reviews three sol-gel-derived liquid entities: Liquid marbles, Liquid plasticine, and nanoparticle-coated flat interface. Liquid marble, a particle-covered droplet, was significantly explored for its application as a container in many biological and chemical processes. Unlike powder-derived liquid marble, sol-gel-derived liquid marble can be formed into any desired shape, commonly known as liquid plasticine. Monolayer-covered sol-gel entities also offer a simple physical platform for investigating many fundamental properties of particle-coated interfaces. In the present review, starting from its preparation to the application, all critical aspects are summarized. Some unaddressed issues compared to the powder LM are also discussed for future research.
Polypyrrole synthesized by solvent-free chemical oxidative polymerization, followed by purification using alkyl alcohols, showed higher C/N atomic ratios and higher hydrophobicity, compared with that synthesized by aqueous chemical oxidative polymerization. The alcohols could function as a hydrophobizer for polypyrrole by physical adsorption and possible chemical adsorption via nucleophilic attack of the alcohol.
Post‐assembly modifications are efficient tools to adjust colloidal features of block copolymer (BCP) particles. However, existing methods often address particle shape, morphology, and chemical functionality individually. For simultaneous control, we transferred the concept of seeded polymerization to phase separated BCP particles. Key to our approach is the regioselective polymerization of (functional) monomers inside specific BCP domains. This was demonstrated in striped PS‐b‐P2VP ellipsoids. Here, polymerization of styrene preferably occurs in PS domains and increases PS lamellar thickness up to 5‐fold. The resulting asymmetric lamellar morphology also changes the particle shape, i.e., increases the aspect ratio. Using 4‐vinylbenzyl azide as co‐monomer, azides as chemical functionalities can be added selectively to the PS domains. Overall, our simple and versatile method gives access to various multifunctional BCP colloids from a single batch of pre‐formed particles.
Post‐assembly modifications are efficient tools to adjust colloidal features of block copolymer (BCP) particles. However, existing methods often address particle shape, morphology, and chemical functionality individually. For simultaneous control, we transferred the concept of seeded polymerization to phase separated BCP particles. Key to our approach is the regioselective polymerization of (functional) monomers inside specific BCP domains. This was demonstrated in striped PS‐b‐P2VP ellipsoids. Here, polymerization of styrene preferably occurs in PS domains and increases PS lamellar thickness up to 5‐fold. The resulting asymmetric lamellar morphology also changes the particle shape, i.e., increases the aspect ratio. Using 4‐vinylbenzyl azide as co‐monomer, azides as chemical functionalities can be added selectively to the PS domains. Overall, our simple and versatile method gives access to various multifunctional BCP colloids from a single batch of pre‐formed particles.
Near-infrared (NIR) light irradiation induced the transformation of polypyrrole (PPy) to nitrogen-containing carbon (NCC) material due to its light-to-heat photothermal property. The temperature of the PPy increased over 700 °C within a few seconds by the NIR laser irradiation, and elemental microanalysis confirmed the decreases of hydrogen and chloride contents and increases of carbon and nitrogen contents. Monodispersed polystyrene (PS)-core/PPy shell particles (PS/PPy particles) synthesized by aqueous chemical oxidative seeded polymerization were utilized as a precursor toward monodispersed NCC capsules. When the NIR laser was irradiated to the PS/PPy particles, the temperature rose to approximately 300 °C and smoke was generated, indicating that the PS component forming the core was thermally decomposed and vaporized. Scanning electron microscopy studies revealed the successful formation of spherical and highly monodispersed capsules, and Fourier transform infrared spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy studies confirmed the capsules consisted of NCC materials. Furthermore, sunlight was also demonstrated to work as a light source to fabricate NCC capsules. The size and thickness of the capsules can be controlled between 1 and 80 μm and 146 and 231 nm, respectively, by tuning the size of the original PS/PPy particles and PPy shell thickness.
Poly(alkylaniline) grains with several tens micrometer-sized diameter were successfully synthesized by aqueous chemical oxidative polymerization. The grains were aggregates consisting of submicrometer sized-atypical particles, which was confirmed by scanning electron microscopy studies. Static contact angle measurements of water droplets on the compressed pellets of the grains indicated that the hydrophobicity increased with an increase of alkyl group length and the alkyl groups bonded to phenyl ring is expected to be exposed to air phase. The data obtained through thermography indicated the grains showed near infrared light-to-heat photothermal property. The dried grains could work as an effective liquid marble stabilizer by efficient adsorption to air-water interface. The remote locomotion control of liquid marble could be attained by near-infrared light-induced Marangoni flow. Furthermore, the liquid marbles could detect oil contamination on water surface by disruption.
A liquid marble (LM) describes a liquid droplet that is wrapped by nonwetting micro- or nanoparticles and therefore obtains characteristics of a solid powder particle. Here, we investigate the effect of the stabilizing particle size on the resulting structure and properties of the LM. We synthesize a series of polystyrene particles with ultrathin coatings of heptadecafluorooctanesulfonic acid-doped polypyrrole with diameters ranging between 1 and 1000 μm by an aqueous chemical oxidative seeded polymerization of pyrrole. The methodology produced a set of hydrophobic particles with similar surface characteristics to allow the formation of LMs and to probe size effects in the LM formation and stabilization efficiency. We found that particles with a size above 20 μm adsorb as a particle monolayer to the surface of the LM, while smaller particles are adsorbed as ill-defined, multilayered aggregates. These results indicate that the balance between particle-particle interaction and gravity is an important parameter to control the surface structure of the LMs. The assembly behavior and size of the particles also correlated with the mechanical integrity of the LM against fall impact. The mechanical resistance was affected by the gap distance between the inner liquid of the LM and supporting substrate, the capillary forces acting between the particles at the LM surface, and the potential energy that depended on the particle size. Last, we demonstrate that the broadband light-absorbing properties of the polypyrrole shell also allow manipulating the evaporation rate of the inner liquid.
