Experimental Investigation of Cavitation Bulk Nanobubbles Characteristics: Effects of pH and Surface-Active Agents.

Nanobubbles (NBs) have a widespread application in antimicrobial activity, wastewater treatment, and ecological restoration due to numerous peculiar characteristics, such as small diameter, long-term stability, and ability to produce hydroxyl radicals. Despite significant applications, only limited comprehensive investigations are available on the role of surfactants and pH in NBs characteristics. Therefore, this study examines the effects of different surfactants (i.e., anionic, cationic, and nonionic) and pH medium on bulk NB formation, diameter, concentration, bubble size distribution (BSD), ζ-potential, and stability. The effect of surfactant at concentrations above and below the critical micelle concentration was investigated. NBs were generated in deionized (DI) water using a piezoelectric transducer. The stability of NBs was assessed by tracking the variation in diameter and concentration over time. In a neutral medium, the diameter of NBs is smaller than in other surfactant or pH mediums. The diameter, concentration, BSD, and stability of NBs are strongly influenced by the ζ-potential rather than the solution medium. BSD curve shifts to a smaller bubble diameter when the magnitude of ζ-potential is high in any solution. In pure water, surfactant, and pH mediums, NBs have existed for a long time. NBs have a shorter life span in environments with a pH ≤ 3. Surfactant adsorption on the surface of NBs increases with increasing surfactant concentration up to a certain limit, beyond which it declines substantially. The Derjaguin-Landau-Verwey-Overbeek (DLVO) theory was used to interpret the NBs stability, resulting in a total potential energy barrier that is positive and greater than 45.55 kBT for 6 ≤ pH ≤ 11, whereas for pH < 6, the potential energy barrier essentially vanishes. Moreover, an effort has also been made to explicate the plausible prospect of ion distribution and its alignment surrounding NBs in cationic and anionic surfactants. This study will extend the in-depth investigation of NBs for industrial applications involving NBs.

Self-Assembled Monolayers Coated Porous SnO2 Film Gas Sensor with Reduced Humidity Influence.

Metal-oxide sensors, detect gas through the reaction of surface oxygen molecules with target gases, are promising for the detection of toxic pollutant gases, combustible gases, and organic vapors; however, their sensitivity, selectivity, and long-term stability limit practical applications. Porous structure for increasing surface area, adding catalyst, and altering the operation temperature are proposed for enhancing the sensitivity and selectivity. Although humidity can significantly affect the property and stability of the sensors, studies focusing on the long-term stability of gas sensors are scarce. To reduce the effects of humidity, 1H, 1H, 2H, 2H-perfluorooctyltriethoxysilane (PFOTS) was coated on a porous SnO2 film. The interconnected SnO2 nanowires improved the high surface area, and the PFOTS coating provided superhydrophobicity at water contact angle of 159°and perfect water vapor repellency inside E-SEM. The superhydrophobic porous morphology was maintained under relative humidity of 99% and operating temperature of 300 °C. The CO gas sensing of 5, 20, and 50 ppm were obtained with linearity at various humidity. Flame detection was also achieved with practical high humidity conditions. These results suggest the simple way for reliable sensing of nanostructured metal-oxide gas sensors with high sensitivity and long-term stability even in highly humid environments.

Controlling the Release of Amphiphilic Liposomes from Alginate Hydrogel Particles for Antifouling Paint.

As an alternative to the toxic antifouling paint that minimizes the adhesion force between organic molecules on large surfaces, a paint containing hydrogel particles encapsulating amphiphilic liposomes has been suggested. However, the release rate of liposomes, which is important for maximizing the antifouling performance, has not been adequately explored. We investigated the control of the release rate of liposomes encapsulated in alginate. Monodispersed alginate particles were generated using 3D-printed microfluidic devices, and their sizes were varied through the channel size, flow rate, and alginate concentration in the microfluidic devices ([Formula: see text]). The release rate of liposomes from the alginate particles was experimentally monitored under various conditions: alginate concentration, surrounding solution, and ambient fluid flow. The effects of chemical and mechanical stimuli on the effective diffusion coefficient (Deff) of amphiphilic liposomes were analyzed, and accordingly, the best production conditions for antifouling alginate particles are suggested. This study provides essential physical insights and is useful for optimizing the performance of eco-friendly antifouling paint that includes alginate particles.

Breakups of an encapsulated surfactant-laden aqueous droplet under a DC electric field.

We investigate the breakups of an encapsulated conducting aqueous droplet under a direct-current electric field via extensive experiments and theoretical analysis. The encapsulating shell phase and the ambient phase consist of leaky dielectric liquids. We change the surface tension by using an aqueous core with different surfactant (Tween 80) concentrations. Moreover, we vary the core size under different electric-field conditions and observe the core dynamics. We present three different breakup modes of the encapsulated droplet. In the first mode, the encapsulated core forms asymmetric Janus shapes after breakup. In the second and third breakup modes, stable and unstable ternary droplets are formed, respectively. We show that the surfactant molecules significantly alter the dynamics of core stretching. According to the theoretical analysis, we identify the critical conditions of instability leading to breakup. We plot the breakup modes in the form of a phase diagram in the electric capillary number (Ca23 = ε3rsEo2/γ23; ratio of interfacial electric to capillary stresses) vs. radius ratio of the core to the shell (ß = rc/rs) parametric space at different nondimensional surfactant concentrations (C* = CTween 80/CCMC, where CCMC represents the critical micellar concentration). The study provides essential physical insight into encapsulated emulsions and is useful for their application in various areas of science and technology.

Multimodal breakup of a double emulsion droplet under an electric field.

We investigate the hydrodynamic deformation and breakup of double emulsion droplets under a uniform DC electric field. Based on comprehensive experiments, we observe four different breakup modes for the double emulsion droplet by varying the viscosity of shell liquid, and conductivity, permittivity or volume fraction of the core liquid. The breakup modes are classified as a unidirectional breakup mode, two different bidirectional breakup modes, and a tip-streaming breakup mode. We performed scaling analysis and numerical simulation to explain the experimental observations. We believe that this study could provide insight for the comprehension of double emulsion droplet functionalities in various applications, including drug delivery, materials science, biological and chemical engineering, and lab-on-a-chip applications.

Mono-emulsion droplet stretching under direct current electric field.

We study the mechanism of stretching and breaking of a mono-emulsion droplet under a direct current electric field using theoretical and experimental approaches aided by numerical simulation. Axisymmetric straining flow driven by an electric field results in the equilibrium deformation of the droplet along the direction of the electric field if the electric capillary number Cae that is the ratio of electric stresses to capillary stresses, is less than a critical value (Cae)crit. At (Cae)crit, the droplet breaks either before showing the slow deformation stage or rapidly. Furthermore, we developed a theoretical model to understand the mechanism of the transition from equilibrium deformation to non-equilibrium breaking. The Cae that can induce Taylor's deformation D = (α - ß)/(α + ß) ≈ 0.295; where α and ß are the lengths of semi-major and semi-minor axes of the droplet, corresponds to (Cae)crit. At this stage, the maximum flow velocity shifts to the outside of the droplet along the electric field direction and large electric stresses are mainly concentrated at the droplet's side apex causing daughter droplet ejection. Finally, we compare the values of (Cae)crit obtained from the theoretical model ((Cae)crit ≈ 0.25) for which the conductivity ratio (R) between the droplet and ambient liquid i.e., R ∼ O(10) with our experimental results ((Cae)crit ≈ 0.245) and realize that (Cae)crit decreases as R increases. We also observe that even though the viscosity ratio can alter the emulsion breakup modes, it has no effect on (Cae)crit for the onset of breaking.

Fabrication, Flow Control, and Applications of Microfluidic Paper-Based Analytical Devices.

Paper-based microfluidic devices have advanced significantly in recent years as they are affordable, automated with capillary action, portable, and biodegradable diagnostic platforms for a variety of health, environmental, and food quality applications. In terms of commercialization, however, paper-based microfluidics still have to overcome significant challenges to become an authentic point-of-care testing format with the advanced capabilities of analyte purification, multiplex analysis, quantification, and detection with high sensitivity and selectivity. Moreover, fluid flow manipulation for multistep integration, which involves valving and flow velocity control, is also a critical parameter to achieve high-performance devices. Considering these limitations, the aim of this review is to (i) comprehensively analyze the fabrication techniques of microfluidic paper-based analytical devices, (ii) provide a theoretical background and various methods for fluid flow manipulation, and iii) highlight the recent detection techniques developed for various applications, including their advantages and disadvantages.

Reverse capillary flow of condensed water through aligned multiwalled carbon nanotubes.

Molecular transport through nanopores has recently received considerable attention as a result of advances in nanofabrication and nanomaterial synthesis technologies. Surprisingly, water transport investigations through carbon nanochannels resulted in two contradicting observations: extremely fast transport or rejection of water molecules. In this paper, we elucidate the mechanism of impeded water vapor transport through the interstitial space of aligned multiwalled carbon nanotubes (aligned-MWCNTs)--capillary condensation, agglomeration, reverse capillary flow, and removal by superhydrophobicity at the tip of the nanotubes. The origin of separation comes from the water's phase change from gas to liquid, followed by reverse capillary flow. First, the saturation water vapor pressure is decreased in a confined space, which is favorable for the phase change of incoming water vapor into liquid drops. Once continuous water meniscus is formed between the nanotubes by the adsoprtion and agglomeration of water molecules, a high reverse Laplace pressure is induced in the mushroom-shaped liquid meniscus at the entry region of the aligned-MWCNTs. The reverse Laplace pressure can be significantly enhanced by decreasing the pore size. Finally, the droplets pushed backward by the reverse Laplace pressure can be removed by superhydrophobicity at the tip of the aligned-MWCNTs. The analytical analysis was also supported by experiments carried out using 4 mm-long aligned-MWCNTs with different intertube distances. The water rejection rate and the separation factor increased as the intertube distance decreased, resulting in 90% and 10, respectively, at an intertube distance of 4 nm. This mechanism and nanotube membrane may be useful for energy-efficient water vapor separation and dehumidification.

Dynamics of a capillary invasion in a closed-end capillary.

The position of fluid invasion in an open capillary increases as the square root of time and ceases when the capillary and hydrostatic forces are balanced, when viscous and inertia terms are negligible. Although this fluid invasion into open-end capillaries has been well described, detailed studies of fluid invasion in closed-end capillaries have not been explored thoroughly. Thus, we demonstrated, both theoretically and experimentally, a fluid invasion in closed-end capillaries, where the movement of the meniscus and the invasion velocity are accompanied by adiabatic gas compression inside the capillary. Theoretically, we found the fluid oscillations during invasion at short time scales by solving the one-dimensional momentum balance. This oscillatory motion is evaluated to determine which physical forces dominate the different conditions, and is further described by a damped driven harmonic oscillator model. However, this oscillating motion is not observed in the experiments. This inconsistency is due to the following: first, a continuous decrease in the radius of the curvature caused by decreasing the invasion velocity and increasing pressure inside the closed-end capillary, and second, the shear stress increase in the short time scale by the plug like velocity profile within the entrance length. The viscous term of modified momentum equation can be written as K(8µl/rc(2))(dl/dt) by using the multiplying factor K, which represents the increase of shear stress. The K is 7.3, 5.1, and 4.8 while capillary aspect ratio χc is 740, 1008, and 1244, respectively.

Homogeneous percolation versus arrested phase separation in attractively-driven nanoemulsion colloidal gels.

We elucidate mechanisms for colloidal gelation of attractive nanoemulsions depending on the volume fraction (ϕ) of the colloid. Combining detailed neutron scattering, cryo-transmission electron microscopy and rheological measurements, we demonstrate that gelation proceeds by either of two distinct pathways. For ϕ sufficiently lower than 0.23, gels exhibit homogeneous fractal microstructure, with a broad gel transition resulting from the formation and subsequent percolation of droplet-droplet clusters. In these cases, the gel point measured by rheology corresponds precisely to arrest of the fractal microstructure, and the nonlinear rheology of the gel is characterized by a single yielding process. By contrast, gelation for ϕ sufficiently higher than 0.23 is characterized by an abrupt transition from dispersed droplets to dense clusters with significant long-range correlations well-described by a model for phase separation. The latter phenomenon manifests itself as micron-scale "pores" within the droplet network, and the nonlinear rheology is characterized by a broad yielding transition. Our studies reinforce the similarity of nanoemulsions to solid particulates, and identify important qualitative differences between the microstructure and viscoelastic properties of colloidal gels formed by homogeneous percolation and those formed by phase separation.

Environmental aluminum oxide inducing neurodegeneration in human neurovascular unit with immunity.

Aluminum oxide nanoparticle (AlNP), a ubiquitous neurotoxin highly enriched in air pollution, is often produced as an inevitable byproduct in the manufacturing of industrial products such as cosmetics and metal materials. Meanwhile, ALNP has emerged as a significant public health concern due to its potential association with neurological diseases. However, the studies about the neurotoxic effects of AlNP are limited, partially due to the lack of physiologically relevant human neurovascular unit with innate immunity (hNVUI). Here, we employed our AlNP-treated hNVUI model to investigate the underlying mechanism of AlNP-driven neurodegeneration. First, we validated the penetration of AlNP across a blood-brain barrier (BBB) compartment and found AlNP-derived endothelial cellular senescence through the p16 and p53/p21 pathways. Our study showed that BBB-penetrating AlNP promoted reactive astrocytes, which produced a significant level of reactive oxygen species (ROS). The astrocytic neurotoxic factors caused neuronal damage, including the synaptic impairment, the accumulation of phosphoric-tau proteins, and even neuronal death. Our study suggests that AlNP could be a potential environmental risk factor of neurological disorders mediated by neuroinflammation.

Controllable preparation of monodisperse microspheres using geometrically mediated droplet formation in a single mold.

We present a surfactant-free fabrication method for simultaneous generation of monodisperse microspheres with controllable size manner. Droplets that become microspheres by solidification processes are made in a two-step process: capillary rising-induced fluid division and wetting of immiscible fluid in a micromold. Design of the mold geometry and the monomer concentration primarily determines the microsphere size and the size distribution. Furthermore, the synergistic effect of two parameters is able to efficiently manipulate the microsphere sizes from submicrometers to a few hundred micrometers.

Eco-friendly polycaprolactone-bound diatomite filter for the removal of metal ions and micro/nanoplastics from water.

Over the last few decades, pollution levels in aquatic environments due to heavy metal ions and micro/nanoplastics have increased owing to industrial development, causing adverse effects on microorganisms. Adsorbent-based filtration is a well-developed technique for removing contaminants from aquatic environments. However, this technique should be improved from the perspectives of eco-friendliness and cost-effectiveness, as commercial adsorbents require energy-intensive synthesis and post-processing with chelating agents. In this study, an eco-friendly filtration system was developed. This system employs biodegradable, natural materials, such as diatomite to remove metal ions and micro/nanoplastics and polycaprolactone (PCL) to make the free-form shapes. The filter removes metal ions via adsorption and micro/nanoplastics via physical size filtration and adsorption. This PCL-bound diatomite filter was fabricated from a mixture of acetone, PCL, and diatomite, varying its size, thickness, shape, and stacking number for a particular objective and usage. The adsorption capacity, kinetics, and permeation flux of the membrane were measured, and the stacking number of the membranes were optimized to maximize the removal efficiency of the target contaminants. This filter is completely biodegradable, as indicated by the degradation of the PCL binder within 60 days in water, without any treatment. The degradable, eco-friendly PCL-bound diatomite filter is a low-cost and sustainable component that can be utilized in various applications, especially potable drinking water production from river in developing country and filtering the micro/nanoplastics from the commercially bottled drinking water in daily life.

Development of in-vitro pulsatile flow generator for evaluating the performance of hemodialysis catheters.

Hemodialysis (HD) using an HD catheter is performed widely on renal failure patients. The catheter was evaluated using the recirculation ratio in pre-clinical status, which is a crucial index indicating its performance. However, pre-clinical in-vivo experiments have limitations: high cost, and ethical issues. Hence, computational and in-vitro methods have been developed as alternatives. However, computational methods require fluid dynamic knowledge, whereas in-vitro experiments are complicated and expensive. In this study, we developed a pulsatile flow generator to mimic blood flow achieving cost effectiveness and user convenience. The device used iterative learning control, achieving blood flow in the superior and inferior vena cava within a 3.3% error. Furthermore, the recirculation ratios were measured based on two insertion directions and two different external pipe materials to evaluate the catheter regarding patients' posture and blood vessel stiffness. The results provide a better understanding of cardiovascular device performance without complicated and costly pre-clinical tests.

Room temperature roll-to-roll additive manufacturing of polydimethylsiloxane-based centrifugal microfluidic device for on-site isolation of ribonucleic acid from whole blood.

Polymer-based lab-on-a-disc (LoaD) devices for isolating ribonucleic acid (RNA) from whole blood samples have gained considerable attention for accurate biomedical analysis and point-of-care diagnostics. However, the mass production of these devices remains challenging in manufacturing cost and sustainability, primarily due to the utilization of a laser cutter or router computer numerical control (CNC) machine for engraving and cutting plastics in the conventional prototyping process. Herein, we reported the first energy-efficient room-temperature printing-imprinting integrated roll-to-roll manufacturing platform for mass production of a polydimethylsiloxane (PDMS)-based LoaD to on-site isolate ribonucleic acid (RNA) from undiluted blood samples. We significantly reduced energy consumption and eliminated thermal expansion variations between the mold, substrate, and resists by accelerating the PDMS curing time to less than 10 min at room temperature without using heat or ultraviolet radiation. The additive manufacturing technology was applied to fabricate a multi-depth flexible polymer mold that integrated macro (2 mm) and micro-sized (500 µm) features, which overcomes the economic and environmental challenges of conventional molding techniques. Our integrated R2R platform was enabled to print adhesion-promoting films at the first printing unit and continuously in-line imprint with a high replication accuracy (99%) for high-volume manufacturing of a new centrifugal microfluidic chip with an enhancement of mixing performance by integrating an efficient mixing chamber and serpentine micromixer. This research paved the way for scalable green manufacturing of large-volume polymer-based microfluidic devices, often required in real-world sample-driven analytical systems for clinical bioanalysis.

3D printed fluidic swab for COVID-19 testing with improved diagnostic yield and user comfort.

The current standard method of diagnosing coronavirus disease 2019 (COVID-19) involves uncomfortable and invasive nasopharyngeal (NP) sampling using cotton swabs (CS), which can be unsuitable for self-testing. Although mid-turbinate sampling is an alternative, it has a lower diagnostic yield than NP sampling. Nasal wash (NW) has a similar diagnostic yield to NP sampling, but is cumbersome to perform. In this study, we introduce a 3D printed fluidic swab (3DPFS) that enables easy NW sampling for COVID-19 testing with improved diagnostic yield. The 3DPFS comprises a swab head, microchannel, and socket that can be connected to a syringe containing 250 µL of NW solution. The 3DPFS efficiently collects nasal fluid from the surface of the nasal cavity, resulting in higher sensitivity than CS for the detection of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). This was confirmed by both reverse transcription-quantitative polymerase chain reaction (RT-qPCR) and lateral flow assays (LFA) in virus-spiked nasal samples and clinical samples. Additionally, users reported greater comfort when using the 3DPFS compared to CS. These findings suggest that the 3DPFS can improve the performance of COVID-19 testing by facilitating efficient and less painful nasal sample collection.

Diffusiophoresis-enhanced particle deposition for additive manufacturing.

The ability to govern particle assembly in an evaporative-driven additive manufacturing (AM) can realize multi-scale features fundamental to creating printed electronics. However, existing techniques remain challenging and often require templates or contaminating solutes. We explore the control of particle deposition in 3D-printed colloids by diffusiophoresis, a previously unexplored mechanism in multi-scale AM. Diffusiophoresis can introduce spontaneous phoretic particle motion by establishing local solute concentration gradients. We show that diffusiophoresis can play a dominant role in complex evaporative-driven particle assembly, enabling a fundamentally new and versatile control of particle deposition in a multi-scale AM process.

Mobile Efficient Diagnostics of Infectious Diseases via On-Chip RT-qPCR: MEDIC-PCR.

The COVID-19 outbreak has caused public and global health crises. However, the lack of on-site fast, reliable, sensitive, and low-cost reverse transcription polymerase chain reaction (RT-PCR) testing limits early detection, timely isolation, and epidemic prevention and control. Here, the authors report a rapid mobile efficient diagnostics of infectious diseases via on-chip -RT-quantitative PCR (RT-qPCR): MEDIC-PCR. First, the authors use a roll-to-roll printing process to accomplish low-cost carbon-black-based disposable PCR chips that enable rapid LED-induced photothermal PCR cycles. The MEDIC-PCR can perform RT (3 min), and PCR (9 min) steps. Further, the cohort of 89 COVID-19 and 103 non-COVID-19 patients testing is completed by the MEDIC-PCR to show excellent diagnostic accuracy of 97%, sensitivity of 94%, and specificity of 98%. This MEDIC-PCR can contribute to the preventive global health in the face of a future pandemic.

Effects of viscogens on RNA transcription inside reovirus particles.

The dsRNA genome of mammalian reovirus (MRV), like the dsDNA genomes of herpesviruses and many bacteriophages, is packed inside its icosahedral capsid in liquid-crystalline form, with concentrations near or more than 400 mg/ml. Viscosity in such environments must be high, but the relevance of viscosity for the macromolecular processes occurring there remains poorly characterized. Here, we describe the use of simple viscogens, glycerol and sucrose, to examine their effects on RNA transcription inside MRV core particles. Transcription inside MRV cores was strongly inhibited by these agents and to a greater extent than either predicted by theory or exhibited by a nonencapsidated transcriptase, suggesting that RNA transcription inside MRV cores is unusually sensitive to viscogen effects. The elongation phase of transcription was found to be a primary target of this inhibition. Similar results were obtained with particles of a second dsRNA virus, rhesus rotavirus, from a divergent taxonomic subfamily. Polymeric viscogens such as polyethylene glycol also inhibited RNA transcription inside MRV cores, but in a size-limited manner, suggesting that diffusion through channels in the MRV core is required for their activity. Modeling of the data suggested that the inherent intracapsid viscosity of both reo- and rotavirus is indeed high, two to three times the viscosity of water. The capacity for quantitative comparisons of intracapsid viscosity and effects of viscogens on macromolecular processes in confined spaces should be similarly informative in other systems.

Shear free and blotless cryo-TEM imaging: a new method for probing early evolution of nanostructures.

Cryogenic transmission electron microscopy (cryo-TEM) is a powerful method to image native state morphologies of nanoscale soft and hard objects suspended in solvents. Sample preparation is a critical step toward producing images at length and time scales of interest. We demonstrate a nearly shear-free sample thinning method which simultaneously allows imaging of evolving nanostructures at subsecond time scales. This device breaks the trade-off between high shear and short time scales typical in current cryo-TEM sample preparation methods. We demonstrate the low-shear feature of the new method by imaging wormlike micelles, showing an interconnected network, in contrast to the traditional sample preparation method which shows aligned micelles at similar time points. The time resolution of this method is demonstrated by imaging morphologies of calcium carbonate (formed through the reaction of calcium chloride with sodium carbonate) at subsecond time scales, capturing its evolution from an amorphous to a crystalline state. The impact of hyperbranched polyglycerol additives on the amorphous to crystalline transition in calcium carbonate at short times is examined. Early images at low shear provide unique fundamental insights into mechanisms of nanostructure evolution, thus offering a new paradigm for research in materials sciences, soft matter, and biological sciences.