Stratified films offer high performance and multifunctionality, yet achieving fully stratified films remains a challenge. The layer-by-layer method, involving the sequential deposition of each layer, has been commonly utilized for stratified film fabrication. However, this approach is time-consuming, labor-intensive, and prone to leaving defects within the film. Alternatively, the self-stratification process exploiting a drying binary colloidal mixture is intensively developed recently, but it relies on strict operating conditions, typically yielding a heterogeneous interlayer. In this study, an active interfacial stratification process for creating completely stratified nanoparticle (NP) films is introduced. The technique leverages NPs with varying interfacial activity at the air-water interface. With the help of depletion pressure, the lateral compression of NP mixtures at the interface induces individual desorption of less interfacial active NPs into the subphase, while more interfacial active NPs remain at the interface. This simple compression leads to nearly perfect stratified NP films with controllability, universality, and scalability. Combined with a solvent annealing process, the active stratification process enables the fabrication of stratified films comprising a polymeric layer atop a NP layer. This work provides insightful implications for designing drug encapsulation and controlled release, as well as manufacturing transparent and flexible electrodes.

Zeta potential refers to the electrokinetic potential present in colloidal systems, exerting significant influence on the diverse properties of nano-drug delivery systems. The impact of the dielectric constant on the zeta potential and charge inversion of highly charged colloidal particles immersed in a variety of solvents spanning from polar, such as water, to nonpolar solvents and in the presence of multivalent salts was investigated through primitive Monte Carlo (MC) model simulations. Zeta potential, ξ, is decreased with the decreasing dielectric constant of the solvent and upon further increase in the salinity and the valency of the salt. At elevated levels of salt, the colloidal particles become overcharged in all solvents. As a result, their apparent charge becomes opposite in sign to the stoichiometric charge. This reversal of charge intensifies until reaching a saturation point with further increase in salinity.

OBJECTIVE: Particle surface chemistry and internal softness are two fundamental parameters in governing the mechanical properties of dense colloidal suspensions, dictating structure and flow, therefore of interest from materials fabrication to processing.
METHODS: Here, we modulate softness by tuning the crosslinker content of poly(N-isopropylacrylamide) microgels, and we adjust their surface properties by co-polymerization with polyethylene glycol chains, controlling adhesion, friction and fuzziness. We investigate the distinct effects of these parameters on the entire mechanical response from restructuring to complete fluidization of jammed samples at varying packing fractions under large-amplitude oscillatory shear experiments, and we complement rheological data with colloidal-probe atomic force microscopy to unravel variations in the particles\' surface properties.
RESULTS: Our results indicate that surface properties play a fundamental role at smaller packings; decreasing adhesion and friction at contact causes the samples to yield and fluidify in a lower deformation range. Instead, increasing softness or fuzziness has a similar effect at ultra-high densities, making suspensions able to better adapt to the applied shear and reach complete fluidization over a larger deformation range. These findings shed new light on the single-particle parameters governing the mechanical response of dense suspensions subjected to deformation, offering synthetic approaches to design materials with tailored mechanical properties.

In the field of preparing cosmetic formulations, recent advances recommend the usage of excipients derived from biocompatible materials. In this context, the present study aimed to prepare and characterize the curcumin-loaded Pickering emulsion for possible applications in cosmetic formulation. The coconut oil which is often the component of skin care formulations is used as the oily phase. Curcumin, which is well known for absorbing solar radiation, is expected to work synergistically with coconut oil towards improving the sun protection factor (SPF) of the formulation. Additionally, curcumin can also protect the intracellular components through its well-known antioxidant mechanisms. The Pickering emulsion of coconut oil into water was prepared using the composite colloidal particles derived from β-carboxymethyl chitosan (CMC) and Gelatin-A (GA) as the emulsifying agent. The reaction conditions in terms of the weight ratios of CMC and GA, the pH of the reaction medium, the oil volume fraction, and the homogenization speed were optimized to obtain the most stable Pickering emulsion. The obtained systems were physico-chemically characterized by dynamic light scattering, zeta potential, optical microscopy, and rheometric measurements. The final CMC-GA-stabilized emulsion demonstrated an oil droplet size of 100 µm and a SPFspectrophotometric (290-320 nm) value of 8.5 at a curcumin loading of 4 mg/mL. Additionally, the final formulation facilitated the uptake of curcumin into fibroblast (WI26) cells under in vitro conditions. Together, the investigation demonstrates a bio-inspired approach to prepare a curcumin-loaded green Pickering emulsion using biocompatible pharmaceutical grade excipients, which may find utility in cosmetic applications.

Entering an era of miniaturization prompted scientists to explore strategies to assemble colloidal crystals for numerous applications, including photonics. However, wet methods are intrinsically less versatile than dry methods, whereas the manual rubbing method of dry powders has been demonstrated only on sticky elastomeric layers, hindering particle transfer in printing applications and applicability in analytical screening. To address this clear impetus of broad applicability, we explore here the assembly on nonelastomeric, rigid substrates by utilizing the manual rubbing method to rapidly (≈20 s) attain monolayers comprising hexagonal closely packed (HCP) crystals of monodisperse dry powder spherical particles with a diameter ranging from 500 nm to 10 μm using a PDMS stamp. Our findings elucidate that the tribocharging-induced electrostatic attraction, particularly on relatively stiff substrates, and contact mechanics force between particles and substrates are critical contributors to attain large-scale HCP structures on conductive and insulating substrates. The best performance was obtained with polystyrene and PMMA powder, while silica was assembled only in HCP structures on fluorocarbon-coated substrates under zero-humidity conditions. Finally, we successfully demonstrated the assembly of tunable crystal patterns on a wafer-scale with great control on fluorocarbon-coated wafers, which is promising in microelectronics, bead-based assays, sensing, and anticounterfeiting applications.

Inspired by natural swarms, various methods are developed to create artificial magnetic microrobotic collectives. However, these magnetic collectives typically receive identical control inputs from a common external magnetic field, limiting their ability to operate independently. And they often rely on interfaces or boundaries for controlled movement, posing challenges for independent, three-dimensional(3D) navigation of multiple magnetic collectives. To address this challenge, self-assembled microrobotic collectives are proposed that can be selectively actuated in a combination of external magnetic and optical fields. By harnessing both actuation methods, the constraints of single actuation approaches are overcome. The magnetic field excites the self-assembly of colloids and maintains the self-assembled microrobotic collectives without disassembly, while the optical field drives selected microrobotic collectives to perform different tasks. The proposed magnetic-photo microrobotic collectives can achieve independent position and path control in the two-dimensional (2D) plane and 3D space. With this selective control strategy, the microrobotic collectives can cooperate in convection and mixing the dye in a confined space. The results present a systematic approach for realizing selective control of multiple microrobotic collectives, which can address multitasking requirements in complex environments.

Opto-thermoelectric tweezers (OTET), which exploit the thermophoretic matter migration under a light-directed temperature field, present a new platform for manipulating colloidal particles with a wide range of materials, sizes, and shapes. Taking advantage of the entropically favorable photon-phonon conversion in light-absorbing materials and spatial separation of dissolved ions in electrolytes, OTET can manipulate the particles in a low-power and high-resolution fashion. In this mini-review, we summarize the concept, working principles, and applications of OTET. Recent developments of OTET in three-dimensional manipulation and parallel trapping of particles are discussed thoroughly. We further present their initial applications in particle filtration and biological studies. With their future development, OTET are expected to find a wide range of applications in life sciences, nanomedicine, colloidal sciences, photonics, and materials sciences.

Colloidal lignin particles (CLPs) have sparked various intriguing insights toward bio-polymeric materials and triggered many lignin-featured innovative applications. Here, we report a multi-solvent sequential fractionation methodology integrating green solvents of acetone, 1-butanol, and ethanol to fractionate industrial lignin for CLPs fabrication. Through a rationally designed fractionation strategy, multigrade lignin fractions with variable hydroxyl group contents, molecular weights, and high purity were obtained without altering their original chemical structures. CLPs with well-defined morphology, narrow size distribution, excellent thermal stability, and long-term colloidal stability can be obtained by rational selection of lignin fractions. We further elucidated that trace elements (S, N) were reorganized onto the near-surface area of CLPs from lignin fractions during the formation process in the form of -SO42- and -NH2. This work provides a sustainable and efficient strategy for refining industrial lignin into high-quality fractions and an in-depth insight into the CLPs formation process, holding great promise for enriching the existing libraries of colloidal materials.

Single-particle catalysis aims at determining factors that dictate the nanoparticle activity and selectivity. Existing methods often use fluorescent model reactions at low reactant concentrations, operate at low pressures, or rely on plasmonic enhancement effects. Hence, methods to measure single-nanoparticle activity under technically relevant conditions and without fluorescence or other enhancement mechanisms are still lacking. Here, we introduce nanofluidic scattering microscopy of catalytic reactions on single colloidal nanoparticles trapped inside nanofluidic channels to fill this gap. By detecting minuscule refractive index changes in a liquid flushed trough a nanochannel, we demonstrate that local H2O2 concentration changes in water can be accurately measured. Applying this principle, we analyze the H2O2 concentration profiles adjacent to single colloidal Pt nanoparticles during catalytic H2O2 decomposition into O2 and H2O and derive the particles\' individual turnover frequencies from the growth rate of the O2 gas bubbles formed in their respective nanochannel during reaction.

This study focused on the separation, characterization, content determination, and antiviral efficacy research on colloidal particles with different sizes in Maxing Shigan Decoction(MXSG). The mixed colloidal phase of MXSG was initially separated into small colloidal particle segment(S), medium colloidal particle segment(M), and big colloidal particle segment(B) using ultrafiltration. Further fine separation was performed using size-exclusion chromatography. Dynamic light scattering(DLS) and transmission electron microscopy(TEM) were employed to characterize the size and morphology of the separated colloidal particles. UPLC-MS/MS was used to determine the content of ephedrine, amygdalin, glycyrrhizic acid, and the EDTA complexometric titration was used to measure the calcium(Ca~(2+)) content in different colloidal phases. Finally, a respiratory syncytial virus(RSV) infection mouse model was established using intranasal administration. The experimental groups included a blank group, a model group, a ribavirin group, an MXSG group, an S group, an M group, and a B group. Oral administration was given for treatment, and pathological changes in mouse lung tissue and organ indices were evaluated. The results of the study showed that the distribution of ephedrine, amygdalin, glycyrrhizic acid, and Ca~(2+) content was not uniform among different colloidal segments. Among them, the B segment had the highest proportions of the three components, except for Ca~(2+), accounting for 46.35%, 53.72%, and 92.36%, respectively. Size-exclusion chromatography separated colloidal particles with uniform morphology in the size range of 100-500 nm. Compared to the S and M segments, the B segment showed an increased lung index inhibition rate(38.31%), spleen index, and thymus index in RSV-infected mice, and it improved the infiltration of inflammatory cells and lung injury in the lung tissue of mice. The complex components in MXSG form colloidal particles of various sizes and morphologies through heating, and small-molecule active components such as ephedrine, amygdalin, glycyrrhizic acid, and Ca~(2+) participate in the assembly to varying degrees. The main material basis for the antiviral effect of MXSG is the colloidal particles with certain particle sizes formed by the assembly of active components during the heating process.