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The efficient reduction of CO 2 into valuable products is a challenging task in an international context marked by the climate change crisis and the need to move away from fossil fuels. Recently, the use of water microdroplets has emerged as an interesting reaction media where many redox processes which do not occur in conventional solutions take place spontaneously. Indeed, several experimental studies in microdroplets have already been devoted to study the reduction of CO 2 with promising results. The increased reactivity in microdroplets is thought to be linked to unique electrostatic solvation effects at the air-water interface. In the present work, we report a theoretical investigation on this issue for CO 2 using first-principles molecular dynamics simulations. We show that CO 2 is stabilized at the interface, where it can accumulate, and that compared to bulk water solution, its electron capture ability is larger. Our results suggest that reduction of CO 2 might be easier in interface-rich systems such as water microdroplets, which is in line with early experimental data and indicate directions for future laboratory studies. The effect of other relevant factors which could play a role in CO 2 reduction potential is discussed., (© 2024 Wiley-VCH GmbH.)

Magnetic field-directed colloidal interactions offer facile tools for assembly of structures that range from linear chains to multidimensional hierarchical architectures. While the field-driven assembly of colloidal particles has commonly been investigated in unbounded media, a knowledge gap remains concerning such assembly in confined microenvironments. Here, we investigate how confinement of ferromagnetic nanoparticles in microspheres directs their magnetic assembly into hierarchical architectures. Microdroplets from polydimethylsiloxane (PDMS) liquid precursor containing dispersed iron oxide magnetic nanoparticles (MNPs) were placed in a static magnetic field leading to the formation of organized assemblies inside the host droplets. By changing the MNP concentrations, we revealed a sequence of microstructures inside the droplets, ranging from linear chains at a low MNP loading, transitioning to a combination of chains and networked bundles, to solely 3D bundles at high MNP loading. These experimental results were analyzed with the aid of COMSOL simulations where we calculated the potential energy to identify the preferred assembly conformations. The chains at high MNP loading minimized their energy by aggregating laterally to form bundles with their MNP dipoles being out-of-registry. We cured these PDMS droplets to immobilize the assemblies by forming soft microbeads. These microbeads constitute an "interaction toolbox" with different magnetic macroscale responses, which are governed by the structuring of the MNPs and their magnetic polarizability. We show that thanks to their ability to rotate by field-induced torque under a rotating field, these microbeads can be employed in applications such as optical modulators and microrollers.

Liquid aerosols are ubiquitous in nature, and several tools exist to quantify their physicochemical properties. As a measurement science technique, electrochemistry has not played a large role in aerosol analysis because electrochemistry in air is rather difficult. Here, a remarkably simple method is demonstrated to capture and electroanalyze single liquid aerosol particles with radii on the order of single micrometers. An electrochemical cell is constructed by a microwire (cylindrical working electrode) traversing a film of ionic liquid (1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide) that is suspended within a wire loop (reference/counter electrode). An ionic liquid is chosen because the low vapor pressure preserves the film over weeks, vastly improving suspended film electroanalysis. The resultant high surface area allows the suspended ionic liquid cell to act as an aerosol net. Given the hydrophobic nature of the ionic liquid, aqueous aerosol particles do not coalesce into the film. When the liquid aerosols collide with the sufficiently biased microwire (creating a complex boundary: aerosol|wire|ionic liquid|air), the electrochemistry within a single liquid aerosol particle can be interrogated in real-time. The ability to achieve liquid aerosol size distributions for aerosols over 1 µm in radius is demonstrated., (© 2024 The Authors. Small published by Wiley‐VCH GmbH.)

Single-molecule catalysis reflects the heterogeneity of each molecule, providing a unique insight into the complex catalytic mechanism through the statistics of stochastic individuals. However, the present study methods for single-molecule catalysis are either complicated or have low throughput, limiting their rapid acquisition of single-molecule reaction kinetics with statistical significance. Here, a label-free imaging method is developed for the study of single-molecule catalysis in microdroplets with high throughput based on the absorption of the reaction molecules. A wide distribution of the catalytic reaction rate constant value of 238-2026 molecules s -1 is observed from 68 single enzymes. Interestingly, an exponential decayed distribution of the enzyme activity can be clearly observed due to the rapid denaturation of the enzymes. The denaturation mechanism of the Horse Radish Peroxidase (HRP) enzyme is clarified. It is revealed that the denaturation of each enzyme goes through a gradual decay rather than a truncated turn-off process from a single molecule point of view. This absorption-based method can be applied to most of the catalytic reactions with high throughput, which offers an indispensable route for the rapid statistical analysis of various single-molecule catalytic reactions, making it particularly suitable for the acquisition of catalytic kinetics from highly unstable enzymes., (© 2024 Wiley‐VCH GmbH.)

Due to their high surface area and low weight, silica aerogels are ideally suited for several uses, including drug delivery, catalysis, and insulation. Oil-water-oil ( OWO ) double emulsion is a simple and regulated technique for encasing a volatile oil phase in a silica shell to produce hollow silica (SiO 2 ) aerogel particles by using hydrophilic and hydrophobic emulsifiers. In this study, the oil-water-oil ( OWO ) double emulsion method was implemented to synthesize surface-modified hollow silica (SiO 2 ) aerogel particles in a facile and effective way. This investigation mainly focused on the influence of the N-hexane-to-water glass ( OW ) ratio ( r ) in the first emulsion, silica (water glass) content concentration ( x ), and surfactant concentration ( s ) variations. Furthermore, surface modification techniques were utilized to customize the aerogel's characteristics. The X-ray diffraction (XRD) patterns showed no imprints of impurities except SiO 2 . Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images highlight the hollow microstructure of silica particles. Zeta potential was used to determine particle size analysis of hollow silica aerogel particles. The oil-water-oil ( OWO ) double emulsion approach was successfully employed to synthesize surface-modified hollow silica (SiO 2 ) aerogel particles, providing precise control over the particle characteristics. By the influence of the optimization condition, this approach improves the aerogel's potential applications in drug delivery, catalysis, and insulation by enabling surface modifications.

Micrometer-sized compartments play significant roles in driving heterogeneous transformations within atmospheric and biochemical systems as well as providing vehicles for drug delivery and novel reaction environments for the synthesis of industrial chemicals. Many reports now indicate that reaction kinetics are accelerated under microconfinement, for example, in sprays, thin films, droplets, aerosols, and emulsions. These observations are dramatic, posing a challenge to our understanding of chemical reaction mechanisms with potentially significant practical consequences for predicting the complex chemistry in natural systems. Here we introduce the idea of kinetic confinement, which is intended to provide a conceptual backdrop for understanding when and why microdroplet reaction kinetics differ from their macroscale analogs.

The creation of micrometer-sized sheets of silver at the air-water interface by direct deposition of electrospray-generated silver ions (Ag + ) on an aqueous dispersion of reduced graphene oxide (RGO), in ambient conditions, is reported. In the process of electrospray deposition (ESD), an electrohydrodynamic flow is created in the aqueous dispersion, and the graphene sheets assemble, forming a thin film at the air-water interface. The deposited Ag + coalesce to make single-crystalline Ag sheets on top of this assembled graphene layer. Fast neutralization of Ag + forming atomic Ag, combined with their enhanced mobility on graphene surfaces, presumably facilitates the growth of larger Ag clusters. Moreover, restrictions imposed by the interface drive the crystal growth in 2D. By controlling the precursor salt concentration, RGO concentration, deposition time, and ion current, the dimensionality of the Ag sheets can be tuned. These Ag sheets are effective substrates for surface-enhanced Raman spectroscopy (SERS), as demonstrated by the successful detection of methylene blue at nanomolar concentrations., (© 2024 Wiley‐VCH GmbH.)

Interaction between tumor-associated macrophages and tumor cells is crucial for tumor development, metastasis, and the related immune process. However, the macrophages are highly heterogeneous spanning from anti-tumorigenic to pro-tumorigenic, which needs to be understood at the single-cell level. Herein, a sessile microdroplet system designed for monitoring cellular behavior and analyzing intercellular interaction, demonstrated with macrophage-tumor cell pairs is presented. An automatic procedure based on the inkjet printing method is utilized for the precise pairing and co-encapsulation of heterotypic cells within picoliter droplets. The sessile nature of microdroplets ensures controlled fusion and provides stable environments conducive to adherent cell culture. The nitric oxide generation and morphological changes over incubation are explored to reveal the complicated interactions from a single-cell perspective. The immune response of macrophages under distinct cellular microenvironments is recorded. The results demonstrate that the tumor microenvironment displays a modulating role in polarizing macrophages from anti-tumorigenic into pro-tumorigenic phenotype. The approach provides a versatile and compatible platform to investigate intercellular interaction at the single-cell level, showing promising potential for advancing single-cell behavior studies., (© 2024 Wiley‐VCH GmbH.)

Coalescence-induced condensation droplet jumping has been extensively studied for anti-icing, condensation heat transfer, water harvesting, and self-cleaning. Another phenomenon that is gaining attention for potential enhancements is the self-ejection of individual droplets. However, the mechanism underlying this process remains elusive due to cases in which the abrupt detachment of an interface establishes an initial Laplace pressure difference. In this study, we investigate the self-ejection of individual droplets from uniformly hydrophobic microstructures with divergent geometries. We design, fabricate, and test arrays of truncated, nanostructured, and hydrophobic microcones arranged in a square pattern. High-speed microscopy reveals the dynamics of a single condensation droplet between four cones: after cycles of growth and stopped self-propulsion, the suspended droplet self-ejects without abrupt detachments. Through analytical modeling of the droplet in a conical pore as an approximation, we describe the slow isopressure growth phases and the rapid transients driven by surface energy release once a dynamic configuration is reached. Microcones with uniform wettability, in addition to being easier to fabricate, have the potential to enable the self-ejection of all nucleated droplets with a designed size, promising significant improvements in the aforementioned applications and others.

Water microdroplets (7 to 11 µm average diameter, depending on flow rate) are sprayed in a closed chamber at ambient temperature, whose relative humidity (RH) is controlled. The resulting concentration of ROS (reactive oxygen species) formed in the microdroplets, measured by the amount of hydrogen peroxide (H 2 O 2 ), is determined by nuclear magnetic resonance (NMR) and by spectrofluorimetric assays after the droplets are collected. The results are found to agree closely with one another. In addition, hydrated hydroxyl radical cations (•OH-H 3 O + ) are recorded from the droplets using mass spectrometry and superoxide radical anions (•O 2 - ) and hydroxyl radicals (•OH) by electron paramagnetic resonance spectroscopy. As the RH varies from 15 to 95%, the concentration of H 2 O 2 shows a marked rise by a factor of about 3.5 in going from 15 to 50%, then levels off. By replacing the H 2 O of the sprayed water with deuterium oxide (D 2 O) but keeping the gas surrounding droplets with H 2 O, mass spectrometric analysis of the hydrated hydroxyl radical cations demonstrates that the water in the air plays a dominant role in producing H 2 O 2 and other ROS, which accounts for the variation with RH. As RH increases, the droplet evaporation rate decreases. These two facts help us understand why viruses in droplets both survive better at low RH values, as found in indoor air in the wintertime, and are disinfected more effectively at higher RH values, as found in indoor air in the summertime, thus explaining the recognized seasonality of airborne viral infections., Competing Interests: Competing interests statement:The authors declare no competing interest.

Mechanical properties of biological tissues fundamentally underlie various biological processes and noncontact, local, and microscopic methods can provide fundamental insights. Here, we present an approach for quantifying the local mechanical properties of biological materials at the microscale, based on measuring the spectral shifts of the optical resonances in droplet microcavities. Specifically, the developed method allows for measurements of deformations in dye-doped oil droplets embedded in soft materials or biological tissues with an error of only 1 nm, which in turn enables measurements of anisotropic stress inside tissues as small as a few pN/μm 2 . Furthermore, by applying an external strain, Young's modulus can be measured in the range from 1 Pa to 35 kPa, which covers most human soft tissues. Using multiple droplet microcavities, our approach could enable mapping of stiffness and forces in inhomogeneous soft tissues and could also be applied to in vivo and single-cell experiments. The developed method can potentially lead to insights into the mechanics of biological tissues., Competing Interests: Competing interests statement:The authors declare no competing interest.

Electrospray ionization (ESI) is among the commonly used atmospheric pressure ionization techniques in mass spectrometry (MS). One of the drawbacks of ESI is the formation of divergent plumes composed of polydisperse microdroplets, which lead to low transmission efficiency. Here, we propose a new method to potentially improve the transmission efficiency of ESI, which does not require additional electrical components and complex interface modification. A dielectric plate-made of ceramic-was used in place of a regular metallic sampling cone. Due to the charge accumulation on the dielectric surface, the dielectric layer around the MS orifice distorts the electric field, focusing the charged electrospray cloud towards the MS inlet. The concept was first verified using charge measurement on the dielectric material surface and computational simulation; then, online experiments were carried out to demonstrate the potential of this method in MS applications. In the online experiment, signal enhancements were observed for dielectric plates with different geometries, distances of the electrospray needle axis from the MS inlet, and various compounds. For example, in the case of acetaminophen (15 μM), the signal enhancement was up to 1.82 times (plate B) using the default distance of the electrospray needle axis from the MS inlet ( d = 1.5 mm) and 12.18 times (plate C) using a longer distance ( d = 7 mm).

Using devices with microfluidic channels can allow for precise control over liquids flowing through them. Merging flows of immiscible liquids can create emulsions with highly monodispersed microdroplets within a carrier liquid, which are ideal for miniaturised reaction vessels which can be generated with a high throughput of tens of thousands of droplets per second. Control of the size and composition of these droplets is generally performed by controlling the pumping system pushing the liquids into the device; however, this is an indirect manipulation and inadequate if absolute precision is required in the size or composition of the droplets. In this work, we extend the previous development of image-based closed-loop feedback control over microdroplet generation to allow for the control of not only the size of droplets but also the composition by merging two aqueous flows. The feedback allows direct control over the desired parameters of volume and ratio of the two components over a wide range of ratios and outperforms current techniques in terms of monodispersity in volume and composition. This technique is ideal for situations where precise control over droplets is critical, or where a library of droplets of different concentrations but the same volume is required.

The esterification reaction of different amino acids with methanol catalyzed by H 2 SO 4 was first studied in the small volume of thin films generated by ESI microdroplet deposition. The reaction is promoted by the pneumatic spray of the ESI source and reaches its maximum efficiency at a thin film temperature of 70 °C. Selective esterification of the COOH moiety was demonstrated. Microdroplet size and thin film volume and lifetime are critical parameters that influenced the reaction outcome. As expected, l-tyrosine and l-phenylalanine having aromatic side chain substituents were the most reactive amino acids, reaching absolute yields of around 40-50%. The amino acid esterification catalyzed by H 2 SO 4 in a thin film occurs under synthetic conditions in which the same reaction in the bulk is not observed.

Microfluidics is a highly interdisciplinary field where the integration of deep-learning models has the potential to streamline processes and increase precision and reliability. This study investigates the use of deep-learning methods for the accurate detection and measurement of droplet diameters and the image restoration of low-resolution images. This study demonstrates that the Segment Anything Model (SAM) provides superior detection and reduced droplet diameter error measurement compared to the Circular Hough Transform, which is widely implemented and used in microfluidic imaging. SAM droplet detections prove to be more robust to image quality and microfluidic images with low contrast between the fluid phases. In addition, this work proves that a deep-learning super-resolution network MSRN-BAM can be trained on a dataset comprising of droplets in a flow-focusing microchannel to super-resolve images for scales ×2, ×4, ×6, ×8. Super-resolved images obtain comparable detection and segmentation results to those obtained using high-resolution images. Finally, the potential of deep learning in other computer vision tasks, such as denoising for microfluidic imaging, is shown. The results show that a DnCNN model can denoise effectively microfluidic images with additive Gaussian noise up to σ = 4. This study highlights the potential of employing deep-learning methods for the analysis of microfluidic images.

Flexible droplet transportation and coalescence are significant for lots of applications such as material synthesis and analytical detection. Herein, we present an effective method for controllable droplet transportation and coalescence via thermal fields. The device used for droplet manipulation is composed of a glass substrate with indium tin oxide-made microheaers and a microchannel with two transport branches and a central chamber, and it's manipulated by sequentially powering the microheaters located at the bottom of microchannel. The fluid will be unevenly heated when the microheater is actuated, leading to the formation of thermal buoyancy convection and the decrease of interfacial tension of fluids. Subsequently, the microdroplets can be transported from the inlets of microchannel to the target position by the buoyancy flow-induced Stokes drag. And the droplet migration velocity can be flexibly adjusted by changing the voltage applied on the microheater. After being transported to the center of central chamber, the coalescence behaviors of microdroplets can be triggered if the microheater located at the bottom of central chamber is continuously actuated. The droplet coalescence is the combined effect of decreased fluid interfacial tension, the shortened droplet distance by buoyancy flow and the increased instability of droplet under the elevated temperature. The droplet coalescence efficiency is also related to the voltage of microheater, by increasing the voltage from 3.5 V to 7 V, the needed time for droplet coalescence dramatically decrease from 220s to 1.4 s. Finally, by the droplet coalescence-triggered calcium hydroxide precipitation reaction, we demonstrate the applicability of the droplet manipulation method on specific sample detection. Therefore, this approach used for droplet transportation and coalescence can be attractive for many droplet-based applications such as analytical detection., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Developing a new strategy to improve the self-assembly efficiency of functional assemblies in a confined space and construct hybrid functional materials is a significant and fascinating endeavor. Herein, we present a highly efficient strategy for achieving the supramolecular self-assembly of well-defined metallacages in microdroplets through continuous-flow microfluidic devices. The high efficiency and versatility of this approach are demonstrated by the generation of five representative metallacages in different solvents containing water, DMF, acetonitrile, and methanol in a few minutes with nearly quantitative yields, in contrast to the yields obtained with the hour-scale reaction time in a batch reactor. A ring-opening catalytic reaction of the metallacages was selected as a model reaction for exploring supramolecular catalysis in microdroplets, whereby the catalytic yield was enhanced by 2.22-fold compared to that of the same reaction in the batch reactor. This work illustrates a new promising approach for the self-assembly of supramolecular systems., (© 2023 Wiley-VCH GmbH.)

Currently, coaxial electrohydrodynamic jet (CE-Jet) printing is used as a promising technique for the alternative fabrication of drop-on-demand micro- and nanoscale structures without using a template. Therefore, this paper presents numerical simulation of the DoD CE-Jet process based on a phase field model. Titanium lead zirconate (PZT) and silicone oil were used to verify the numerical simulation and the experiments. The optimized working parameters (i.e., inner liquid flow velocity 150 m/s, pulse voltage 8.0 kV, external fluid velocity 250 m/s, print height 16 cm) were used to control the stability of the CE-Jet, avoiding the bulging effect during experimental study. Consequently, different sized microdroplets with a minimum diameter of ~5.5 µm were directly printed after the removal of the outer solution. The model is considered the easiest to implement and is powerful for the application of flexible printed electronics in advanced manufacturing technology.

Hypothesis: Droplet spreading governs various daily phenomena and industrial processes. Insights about microdroplet spreading are limited due to experimental difficulties arising from microdroplet manipulation and substrate wettability control. For droplet sizes approaching the capillary length scale, the gravitational force plays an important role in spreading. In contrast, capillary and viscous forces dominate as the droplet size reduces to smaller length scales. We hypothesize that the dynamic spreading behavior of microdroplets whose radius is far lower than the capillary length differs substantially from established and well understood dynamics., Experiments: To systematically investigate the spreading dynamics of microdroplets, we develop contact-initiated wetting techniques combined with structuring-independent wettability control to achieve microdroplet (<500 μm) spreading on arbitrary surfaces while eliminating parasitic pinning effects (pining force ∼ 0) and initial impact momentum effects (Weber number ∼ 0)., Findings: Our experiments reveal that the capillary-driven initial spreading of microdroplets is shorter, with significantly reduced oscillation dampening, when compared to millimeter-scale droplets. Furthermore, spreading along with capillary wave propagation results in coupling between the spreading velocity and dynamic contact angle at the contact line. These findings, along with our proposed microdroplet manipulation platform, may find application in microscale heat transfer, advanced manufacturing, and aerosol transmission studies., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Inc. All rights reserved.)

This work reports the formation of silver nanoparticles (AgNPs) by sputter deposition in thin films of three different ionic liquids (ILs) with the same anion (bis(trifluoromethylsulfonyl)imide) and cation (imidazolium), but with different alkyl chain lengths and symmetries in the cationic moiety ([C 4 C 1 im][NTf 2 ], [C 2 C 2 im][NTf 2 ], and [C 5 C 5 im][NTf 2 ]). Ionic liquid (IL) films in the form of microdroplets with different thicknesses (200 to 800 monolayers) were obtained through vacuum thermal evaporation onto glass substrates coated with indium tin oxide (ITO). The sputtering process of the Ag onto the ILs when conducted simultaneously with argon plasma promoted the coalescence of the ILs' droplets and the formation, incorporation, and stabilization of the metallic nanoparticles in the coalesced IL films. The formation/stabilization of the AgNPs in the IL films was confirmed using high-resolution scanning electron microscopy (SEM) and UV-Vis spectroscopy. It was found that the IL films with larger thicknesses (600 and 800 monolayers) were better media for the formation of AgNPs. Among the ILs used, [C 5 C 5 im][NTf 2 ] was found to be particularly promising for the stabilization of AgNPs. The use of larger IL droplets as capture media was found to promote a better stabilization of the AgNPs, thereby reducing their tendency to aggregate.

Microcapsules with a liquid core and a solid shell composed of hydrophobic nanoparticles are broadly applied in food, pharmaceutics, and biotechnologies. For example, Pickering emulsions, colloidosomes, or antibubbles (droplets surrounded by air layers in water) enable controlled release of active agents, biocompatibility, and contact-less liquid transportation. However, producing controlled nanoparticle- or polymer-laden hydrophobic shells at scale is highly challenging, since bulk methods are polydisperse and microfluidic chips are prone to clogging and slow. Here, clog-free coating of an aqueous jet with silica nanoparticle suspensions with concentrations up to 10% (w/v), as well as high concentrations of polymers (30% (w/v) poly(lactic acid) (PLA)), is demonstrated, enabling continuous generation of microcapsules at flow rates up to 4 mL min -1 . Pickering emulsions are converted into capsules, providing hydrophobic shells consisting of nanoparticles for controlled release. As a highlight, the scalable fabrication of air-coated capsules (antibubbles) in the sub-millimeter range is demonstrated. The shell contains an air film that protects the liquid core for days yet enables ultrasound-induced release within 3 min. By enabling rapid fabrication of controlled Pickering emulsions, colloidosomes, antibubbles, and biodegradable capsules, jetting through a liquid layer (JetALL) provides a versatile platform for advanced applications in food, pharmacy, and life science., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

We present immunoassay-based desorption electrospray ionization mass spectrometry imaging (immuno-DESI-MSI) to visualize functional macromolecules such as drug targets and cascade signaling factors. A set of boronic acid mass tags (BMTs) were synthesized to label antibodies as MSI probes. The boronic ester bond is employed to cross-link the BMT with the galactosamine-modified antibody. The BMT can be released from its tethered antibody by ultrafast cleavage of the boronic ester bond caused by the acidic condition of sprayed DESI microdroplets containing water. The fluorescent moiety enables the BMT to work in both optical and MS imaging modes. The positively charged quaternary ammonium group enhances the ionization efficiency. The introduction of the boron element also makes mass tags readily identified because of its unique isotope pattern. Immuno-DESI-MSI provides an appealing strategy to spatially map macromolecules beyond what can be observed by conventional DESI-MSI, provided antibodies are available to the targeted molecules of interest., (© 2023 Wiley-VCH GmbH.)

Due to their important roles in medicine and asymmetric metal catalysis, the formation of Betti bases has attracted wide interest in organic chemical community. Traditional multicomponent reaction methods for synthesizing Betti bases normally require long reaction times under harsh conditions (high temperature, microwave or ultrasonic irradiation, etc.) in the presence of various catalysts. In this study, we developed a mild, highly efficient and environmentally friendly method to synthesize Betti bases without the use of any catalysts in microdroplets. The Betti reaction was accelerated by 6.53×10 3 in microdroplets by comparing the measured rate constant in bulk. Fifteen Betti bases were synthesized by the microdroplet method using a variety of aldehydes, naphthols and amines with 68-98 % yields at a scaled-up amount of 1.9 g h -1 . Overall it is an attractive alternative to classic organic synthesis for the construction of Betti bases and derivatives., (© 2022 Wiley-VCH GmbH.)

The delivery of lipophilic dyes, such as BODIPY 505/515, to cells is often hindered by their low aqueous solubility, necessitating the use of organic solvents to facilitate the delivery, which unfortunately compromises the viability of the cells. In this work, we demonstrate the generation of novel composite hydrogel microparticles loaded with BODIPY 505/515, which can be used to deliver the dye to microalgal cells to stain the intracellular lipids. The microparticles were prepared by combining polymeric micelles with hydrogel technology to obtain microparticles of enhanced loading capacity. The generated hydrogel microparticles were tested by incubation with Phaeodactylum tricornutum algal cells. The cells were rapidly and successfully stained by the dye-containing microparticles, and their viability was not affected by the staining process. The method can also be used to stain other types of microalgal cells, such as Nannochloropsis gaditana cells. We therefore believe that this work offers a versatile and useful solution to important cell-staining problems in biotechnology., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

We present an integrated droplet-based microfluidic platform for high-throughput protein crystallization experimentation. The device consists of commercially available micro-junctions and PFA tubing assembled for different functions: droplet generation, incubation, and observation. Herein, we describe a complete methodology to generate hundreds of droplets with controlled properties (i.e., size, generation frequency, and composition). Therefore, multiple trials can be carried out under controlled experimental conditions for the screening and optimization of protein crystallization conditions., (© 2023. The Author(s), under exclusive license to Springer Science+Business Media, LLC, part of Springer Nature.)

This work focuses on identifying and prioritizing factors that allow control of the properties of polyelectrolyte-surfactant complexes in two-phase microfluidic confinement and provide advantages over synthesis of such complexes in macroscopic conditions. We characterize the impact of polymer and surfactant aqueous flow conditions on the formation of microscale droplets and fluid threads in the presence of an immiscible organic solvent. We perform an experimental and selected numerical analysis of fast supramolecular reactions in droplets and threads. The work offers a quantitative control over properties of polyelectrolyte-surfactant complexes produced in two-phase confinement by varying capillary numbers and the ratio of aqueous and organic flowrates. We propose a combined thread-droplet mode to synthesize polyelectrolyte-surfactant complexes. This mode allows the production of complexes in a broader size range of R ≈ 70-200 nm, as compared with synthesis in macroscopic conditions and the respective sizes R ≈ 100-120 nm. Due to a minimized impact of undesirable post-chip reactions and ordered microfluidic confinement conditions, the dispersity of microfluidic aggregates (PDI = 0.2-0.25) is lower than that of their analogs synthesized in bulk (PDI = 0.3-0.4). The proposed approach can be used for tailored synthesis of target drug delivery polyelectrolyte-surfactant systems in lab-on-chip devices for biomedical applications., Competing Interests: The authors declare no conflict of interest.

Microdroplets show unique chemistry, especially in their intrinsic redox properties, and to this we here add a case of simultaneous and spontaneous oxidation and reduction. We report the concurrent conversions of several phosphonates to phosphonic acids by reduction (R-P → H-P) and to pentavalent phosphoric acids by oxidation. The experimental results suggest that the active reagent is the water radical cation/anion pair. The water radical cation is observed directly as the ionized water dimer while the water radical anion is only seen indirectly though the spontaneous reduction of carbon dioxide to formate. The coexistence of oxidative and reductive species in turn supports the proposal of a double-layer structure at the microdroplet surface, where the water radical cation and radical anion are separated and accumulated., (© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Existing preparation methods for microdroplets usually require offline measurements to characterize single microdroplets. Here, we report an optical method used to facilitate the controllable formation and real-time characterization of single microdroplets. The optical tweezer technique was used to capture and form a microdroplet at the center of the trap. The controllable growth and real-time characterization of the microdroplet was realized, respectively, by adjusting experimental parameters and by resolving the Raman spectra by fitting Mie scattering to the spike positions of the spectra during the controllable growth of microdroplets. The proposed method can be potentially applied in optical microlenses and virus detection.

Single-particle inductively coupled plasma time-of-flight mass spectrometry (spICP-TOFMS) is a high-throughput method for the multiplexed analysis of nanoparticles (NPs). However, matrix interferences are a significant challenge that must be overcome for accurate NP sizing and number concentration determination. In online microdroplet calibration, multi-element droplet standards are mixed with nebulized aerosols from a NP-containing sample in a dual-sample introduction system before entering the ICP. Microdroplet standards are used to determine absolute sensitivities and calibrate the mass amount(s) of analyte element(s) in particle events. A plasma-uptake standard is added to NP-containing samples to account for variations in the nebulization and transport efficiency of aerosols into the plasma, which are used in the determination of particle number concentrations (PNCs). Since the microdroplets experience the same plasma conditions as analyte NPs, this creates a matrix-matched calibration. We studied the efficacy of online microdroplet calibration for the quantification of NPs in three organic matrices: ethanol, acetone, and acetonitrile. Organic solvents can cause a pronounced increase in sample uptake and cause plasma-related signal attenuation for nanoparticle measurements. Online microdroplet calibration corrects for both effects without the use of nanoparticle standards. Our results demonstrate accurate NP sizing and PNC determinations in organic matrices up to 98% (v/v), even when these matrices caused signals to be attenuated up to 35-times and nebulizer transport efficiencies to be up to four-times higher than that of a pure water matrix., (© 2022. Springer-Verlag GmbH Germany, part of Springer Nature.)

Adhesion and spreading of liquid metals (LMs) on substrates are essential steps for the generation of flexible electronics and thermal management devices. However, the controlled deposition is limited by the high surface tension and peculiar wetting and adhesion behavior of LMs. Herein, we introduce gelatin-regulated LM droplet deposition and sintering (GLMDDS), for the upscalable production of conformally adhesive, solidlike, yet transient LM thin films and patterns on diverse substrates. This method involves four steps: homogeneous deposition of LM microdroplets, gelation of the LM-gelatin solution, toughening of the gelatin hydrogel by solvent displacement, and peeling-induced sintering of LM microdroplets. The LM thin film exhibits a three-layer structure, comprising an LM microdroplet-embedded tough organohydrogel adhesion layer, a continuous LM layer, and an oxide skin. The composite exhibits high stretchability and mechanical robustness, conformal adhesion to various substrates, high conductivity (4.35 × 10 5 S·m -1 ), and transience (86% LM recycled). Large-scale deposition (i.e., 5.6 dm 2 ) and the potential for patterns on diverse substrates demonstrate its upscalability and broad suitability. Finally, the LM thin films and patterns are applied for flexible and wearable devices, i.e., pressure sensors, heaters, human motion tracking devices, and thermal management devices, illustrating the broad applicability of this strategy.

The Maillard reaction kinetics in the confined volume of the thin film produced by ESI microdroplet deposition was studied by mass spectrometry. The almost exclusive formation of the Amadori product from the reaction of D-xylose and D-glucose toward L-glycine and L-lysine was demonstrated. The thin film Maillard reaction occurred at a mild synthetic condition under which the same process in solution was not observed. The comparison of the thin film kinetics with that of the reaction performed in solution showed strong thin film rate acceleration factors.

Amorphous calcium carbonate (ACC) plays an important role in microbially induced calcium carbonate precipitation (MICP), which has great potential in broad applications such as building restoration, CO 2 sequestration, and bioremediation of heavy metals, etc. However, our understanding of ACC is still limited. By combining microscopy of cell-laden microdroplets with confocal Raman microspectroscopy, we investigated the ACC dynamics during MICP. The results show that MICP inside droplets can be divided into three stages: liquid, gel-like ACC, and precipitated CaCO 3 stages. In the liquid stage, the droplets are transparent. As the MICP process continues into the gel-like stage, the ACC structure appears and the droplets become opaque. Subsequently, dissolution of the gel-like structure is accompanied by growth of precipitated CaCO 3 crystals. The size, morphology, and lifetime of the gel-like structures depend on the Ca 2+ concentration. Using polystyrene colloids as tracers, we find that the colloids exhibit diffusive behavior in both the liquid and precipitated CaCO 3 stages, while their motion becomes arrested in the gel-like ACC stage. These results provide direct evidence for the formation-dissolution process of the ACC-formed structure and its gel-like mechanical properties. Our work provides a detailed view of the time evolution of ACC and its mechanical properties at the microscale level, which has been lacking in previous studies.

The quality of indoor air in healthcare facilities, with an emphasis on dental offices, attracted the attention of the scientific community in the late 1960s. Since then, it has become evident that the indoor air quality is critical in modern dental care facilities for limiting the spread of airborne infections, including vaccine-preventable diseases, and a key component of safety for healthcare personnel and patients. In the past decades, the role of indoor air quality has also been recognized in non-healthcare facilities, given the increasing time spent indoors by humans. During the provision of dental care services, mainly in the field of restorative dentistry, high-speed dental handpieces emitting air and water are used, producing large quantities of aerosol and hovering inside the operations area. In modern dental offices, new devices emitting air/powder for cavities improvement and cleaning as well as for periodontal prophylactic cleaning and aesthetics are used. In addition, a new therapeutic protocol for the removal of bacterial biofilm, targeting treatment for peri-implant diseases and conditions using air-abrasive decontamination technology, has been introduced in daily dental practice. The aim of this non-systemic review is to present the current state of knowledge on the nature and dynamics of air splatters and to provide an update to management and control strategies in dental care facilities, focusing on air purification and ultraviolet devices proposed and used. The findings arising from the limited number of related published articles documenting the reduction in levels of particular matter 2.5 (PM 2.5 ), PM 10 and volatile organic compounds, allow us to conclude that the continuous operation of air purifiers during and after treatment, contributes considerably to the improvement of the indoor air quality in dental care facilities. Moreover, the utilization of air purifiers is highly recommended in dental practice to mitigate spread of infections, including vaccine-preventable diseases. Frequent cleaning and maintenance of the purifier sieves and filters and frequent renovation of the indoor air through physical ventilation by mean of open windows is imperative. More research on environmental contamination and particularly on viral contamination under real dental care conditions is needed.

Conventional manufacturing methods for polydimethylsiloxane (PDMS)-based microdevices require multiple steps and elements that increase cost and production time. Also, these PDMS microdevices are mostly limited to single use, and it is difficult to recover the contents inside the microchannels or perform advanced microscopy visualization due to their irreversible sealing method. Herein, we developed a novel manufacturing method based on polymethylmethacrylate (PMMA) plates adjusted using a mechanical pressure-based system. One conformation of the PMMA plate assembly system allows the reproducible manufacture of PDMS replicas, reducing the cost since a precise amount of PDMS is used, and the PDMS replicas show uniform dimensions. A second form of assembling the PMMA plates permits pressure-based sealing of the PDMS layer with a glass base. By reversibly sealing the microdevice without using plasma for bonding, we achieve chip on/off configurations, which allow the user to open and close the device and reuse it in an easy-to-use way. No deformation was observed on the structures of the PDMS microchannels when a range of 10 to 18 kPa pressure was applied using the technique. Furthermore, the functionality of the proposed system was successfully validated by the generation of microdroplets with reused microdevices via three repetitions.

Thin films derived by the deposition of charged microdroplets generated in the ESI source of a mass spectrometer act as highly concentrated reaction vessels in which the final products of an ion-molecule reaction can be isolated by their precipitation onto a solid surface under ambient conditions. In this study, the ESI Z-spray source supplied to a Q-TOF Ultima mass spectrometer was used to investigate the d-fructose acid-catalyzed reactions by microdroplets deposition onto a stainless-steel target surface. High conversion ratios of d-fructose into 5-hydroxymethylfuraldehyde (5-HMF), 5-methoxymethylfuraldehyde (5-MMF), and difructrose anhydrides (DFAs) were obtained with HCl and KHSO 4 as metal-free catalysts by using synthetic conditions under which the same products in bulk are not formed. Furthermore, the reaction outcome was found to be highly sensitive to the catalyst and the solvent employed as well as to the ESI source parameters influencing the thin film formation from microdroplets deposition onto the solid surface.

Purpose: Micron-sized perfluorocarbon droplet adjuvants to focused ultrasound therapies allow lower applied power, circumvent unwanted prefocal heating, and enhance thermal dose in highly perfused tissues. The heat enhancement has been shown to saturate at increasing concentrations. Experiments were performed to empirically model the saturating heating effects during focused ultrasound. Materials and methods: The measurements were made at varying concentrations using magnetic resonance thermometry and focused ultrasound by circulating droplets of mean diameter 1.9 to 2.3 µm through a perfused phantom. A simulation was performed to estimate the interaction radius size, empirically. Results: The interaction radius, representing the radius of a sphere encompassing 90% of the probability for the transformation of acoustic energy into heat deposition around a single droplet, was determined experimentally from ultrasonic absorption coefficient measurements The simulations suggest the interaction radius was approximately 12.5-fold larger than the geometrical radius of droplets, corresponding to an interaction volume on the order of 2000 larger than the geometrical volume. Conclusions: The results provide information regarding the dose-response relationship from the droplets, a measure with 15% precision of their interaction radii with focused ultrasound, and subsequent insights into the underlying physical heating mechanism.

Late-stage functionalization (LSF) of drug molecules is an approach to generate modified molecules that retain functional groups present in the active drugs. Here, we report a study that seeks to characterize the potential value of high-throughput desorption electrospray ionization mass spectrometry (HT DESI-MS) for small-scale rapid LSF. In conventional route screening, HT-based DESI-MS provides contactless, rapid analysis, reliable and reproducible data, minimal sample requirement, and exceptional tolerance to high salt concentrations. Ezetimibe (E), an established hypertension drug, is targeted for modification by LSF. C-H alkenylation and azo-click reactions are utilized to explore this approach to synthesis and analytical characterization. The effect of choice of reactant, stoichiometry, catalyst, and solvent are studied for both reactions using high throughput DESI-MS experiments. Optimum conditions for the formation of LSF products are established with identification by tandem mass spectrometry (MS/MS)., (© 2021 Wiley-VCH GmbH.)

We developed a method for passively controlling microdroplet rotation, including interior rotation, using a parallel flow comprising silicone and sesame oils. This device has a simple 2D structure with a straight channel and T-junctions fabricated from polydimethylsiloxane. A microdroplet that forms upstream moves into the sesame oil. Then, the largest flow velocity at the interface of the two oil layers applies a rotational force to the microdroplet. A microdroplet in the lower oil rotates clockwise while that in the upper oil rotates anti-clockwise. The rotational direction was controlled by a simple combination of sesame and silicone oils. Droplet interior flow was visualized by tracking microbeads inside the microdroplets. This study will contribute to the efficient creation of chiral molecules for pharmaceutical and materials development by controlling rotational direction and speed.

In the aqueous environment, Fe II ions enhance the oxidative potential of ozone and hydrogen peroxide by generating the reactive oxoiron species (ferryl ion, Fe IV O 2+ ) and hydroxyl radical (·OH) via Fenton chemistry. Herein, we investigate factors that control the pathways of these reactive intermediates in the oxidation of dimethyl sulfoxide (Me 2 SO) in Fe II solutions reacting with O 3 in both bulk-phase water and on the surfaces of aqueous microdroplets. Electrospray ionization mass spectrometry is used to quantify the formation of dimethyl sulfone (Me 2 SO 2 , from Fe IV O 2+ + Me 2 SO) and methanesulfonate (MeSO 3 - , from ·OH + Me 2 SO) over a wide range of Fe II and O 3 times faster on microdroplets than that in bulk-phase water. Since the production of MeSO 4 times faster on microdroplets than that in bulk-phase water. Since the production of MeSO 3 - is initiated by ·OH radicals at diffusion-controlled rates, experimental ratios of Me 2 SO 2 /MeSO 3 - > 10 2 suggest that Fe IV O 2+ is the dominant intermediate under all conditions. Me 2 SO 2 yields in the presence of ligands, L, vary as volcano-plot functions of E 0 (LFe IV O 2+ + O 2 /LFe 2+ intermediates in Fenton chemistry taking place on aqueous microdroplets.3 ) reduction potentials calculated by DFT with a maximum achieved in the case of L≡oxalate. Our findings underscore the key role of ferryl Fe IV O 2+ intermediates in Fenton chemistry taking place on aqueous microdroplets.

Isobaric ions having the same mass-to-charge ratio cannot be separately identified by mass spectrometry (MS) alone, but this limitation can be overcome by using hydrogen-deuterium exchange (HDX) in microdroplets. Because isobaric ions may contain a varied number of exchangeable sites and different types of functional groups, each one produces a unique MS spectral pattern after droplet spray HDX without the need for MS/MS experiments or introduction of ion mobility measurements. As an example of the power of this approach, isobaric ions in urinary metabolic profiles are identified and used to distinguish between healthy individuals and those having bladder cancer.

The accelerated formation of 2,3-diphenylquinoxalines in microdroplets generated in a nebulizer has been investigated by competition experiments in which equimolar quantities of 1,2-phenylenediamine, C 6 H 4 (NH 2 ) 2 , and a 4-substituted homologue, XC 6 H 3 (NH 2 ) 2 [X = F, Cl, Br, CH 3 , CH 3 O, CO 2 CH 3 , CF 3 , CN or NO 2 ], or a 4,5-disubstituted homologue, X 2 C 6 H 2 (NH 2 ) 2 [X = F, Cl, Br, or CH 3 ], compete to condense with benzil, (C 6 H 5 CO) 2 . Electron-donating substituents (X = CH 3 and CH 3 O) accelerate the reaction; in contrast, electron-attracting substituents (X = F, Cl, Br and particularly CO 2 CH 3 , CN, CF 3 and NO 2 ) retard it. A structure-reactivity relationship in the form of a Hammett correlation has been found by analyzing the ratio of 2,3-diphenylquinoxaline and the corresponding substituted-2,3-diphenylquinoxaline, giving a ρ value of -0.96, thus confirming that the electron density in the aromatic ring of the phenylenediamine component is reduced in the rate-limiting step in this accelerated condensation. This correlation shows that the phenylenediamine acts as a nucleophile in the reaction.

The application of microfluidic technologies to microalgal research is particularly appealing since these approaches allow the precise control of the extracellular environment and offer a high-throughput approach to studying dynamic cellular processes. To expand the portfolio of applications, here we present a droplet-based microfluidic method for analysis and screening of Phaeodactylum tricornutum and Nannochloropsis gaditana , which can be integrated into a genetic transformation workflow. Following encapsulation of single cells in picolitre-sized droplets, fluorescence signals arising from each cell can be used to assess its phenotypic state. In this work, the chlorophyll fluorescence intensity of each cell was quantified and used to identify populations of P. tricornutum cells grown in different light conditions. Further, individual P. tricornutum or N. gaditana cells engineered to express green fluorescent protein were distinguished and sorted from wild-type cells. This has been exploited as a rapid screen for transformed cells within a population, bypassing a major bottleneck in algal transformation workflows and offering an alternative strategy for the identification of genetically modified strains., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (© 2021 The Authors.)

The development of synthetic systems that enable the sustained active self-assembly of molecular blocks to mimic the complexity and dynamic behavior of living systems is of great interest in elucidating the origins of life, understanding the basic principles behind biological organization, and designing active materials. However, it remains a challenge to construct microsystems with dynamic behaviors and functions that are connected to molecular self-assembly processes driven by external energy. Here, an active self-assembly of microdroplet protocells with dynamic structure and high structural complexity through living radical polymerization under constant energy flux is reported. The active microdroplet protocells exhibit nonlinear behaviors including oscillatory growth and shrinkage. This relies on the transient stabilization of molecular assembly, which can channel the inflow of energy through noncovalent interactions of pure synthetic components. The intercommunication of microdroplet protocells through stochastic fusion leads to the formation of a variety of dynamic and higher-order biomimetic microstructures. This work constitutes an important step toward the realization of autonomous and dynamic microsystems and active materials with life-like properties., (© 2021 Wiley-VCH GmbH.)

The electrochemical formation mechanism of microdroplets formed around a primary droplet of 3.5% NaCl solution on an iron-plated film was investigated by quartz crystal microbalance (QCM) and concentric three-electrode array (CTEA) measurements. During the initial stage, the microdroplets mainly originate from evaporation owing to cathodic polarization and electric current of the localized corrosion cell under the primary droplet. The maximal electrochemical potential difference between the anode and cathode was measured to be 0.36 V and acted as the driving force for the formation of microdroplets. The maximums of anodic and cathodic electric current density of pure iron under the NaCl droplet are 764 and -152 μA/cm 2 , respectively. Propagation of microdroplets in the developing stage attributes to horizontal movement of the electrolyte, water evaporation, and recondensation from primary and capillary condensation from moist air. The results of the study suggest that the initiation and propagation of microdroplets could promote and accelerate marine atmospheric corrosion., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2021 Tang, Li, Wu, Hu, Ma, Li and Fan.)

The use of micrometer-sized droplets for chemical and biochemical analysis has been widely explored. Photolithography is mainly used to fabricate microfluidic devices, which is often employed to form monodisperse microdroplets. Although photolithography enables precise microfabrication, it is not readily available to biochemists because it requires specialized equipment such as clean room and mask aligners, and expensive consumables such as photoresist and silicon wafers. In this study, we fabricated a microfluidic device using a consumer laser cutter and applied it to droplet formation. Monodisperse microdroplets were formed by using an oil phase for droplet digital polymerase chain reaction (PCR) as the continuous phase and phosphate-buffered saline or polyethylene glycol solution as the dispersed phase. The droplet size decreased as the flow rate of the continuous phase increased and approached a constant value. The method developed in this study can be used to realize microdroplet-based biochemical analysis with simple devices or to construct artificial cells.

We previously reported a new approach for micromanipulation and encapsulation of human stem cells using a droplet-based microfluidic device. This approach demonstrated the possibility of encapsulating and culturing difficult-to-preserve primary human hematopoietic stem cells using an engineered double-layered bead composed by an inner layer of alginate and an outer layer of Puramatrix. We also demonstrated the maintenance and expansion of Multiple Myeloma cells in this construction. Here, the presented microfluidic technique is applied to construct a 3D biomimetic model to recapitulate the human hematopoietic stem cell niche using double-layered hydrogel beads cultured in 10% FBS culture medium. In this model, the long-term maintenance of the number of cells and expansion of hHSCS encapsulated in the proposed structures was observed. Additionally, a phenotypic characterization of the human hematopoietic stem cells generated in the presented biomimetic model was performed in order to assess their long-term stemness maintenance. Results indicate that the ex vivo cultured human CD34+ cells from bone marrow were viable, maintained, and expanded over a time span of eight weeks. This novel long-term stem cell culture methodology could represent a novel breakthrough to improve Hematopoietic Progenitor cell Transplant (HPT) as well as a novel tool for further study of the biochemical and biophysical factors influencing stem cell behavior. This technology opens a myriad of new applications as a universal stem cell niche model potentially able to expand other types of cells.

Recently, liquid-liquid phase separation (LLPS) has attracted considerable attention among researchers in the life sciences as a plausible mechanism for the generation of microstructures inside cells. LLPS occurs through multiple nonspecific interactions and does not always require a lock-and-key interaction with a binary macromolecular solution. The remarkable features of LLPS include the non-uniform localization and concentration of solutes, resulting in the ability to isolate certain chemical systems and thereby parallelize multiple chemical reactions within the limited space of a living cell. We report that, by using the macromolecules, poly(ethylene glycol) (PEG) and dextran, that exhibit LLPS in an aqueous solution, cell-sized liposomes are spontaneously formed therein in the presence of phospholipids. In this system, LLPS is generated through the depletion effect of macromolecules. The results showed that cell-like microdroplets entrapping DNA wrapped by a phospholipid layer emerge in a self-organized manner., (© 2020 The Authors. Published by Wiley-VCH GmbH.)

Recently, chemical operations with microfluidic devices, especially droplet-based operations, have attracted considerable attention because they can provide an isolated small-volume reaction field. However, analysis of these operations has been limited mostly to aqueous-phase reactions in water droplets due to device material restrictions. In this study, we have successfully demonstrated droplet formation of five common organic solvents frequently used in chemical synthesis by using a simple silicon/glass-based microfluidic device. When an immiscible liquid with surfactant was used as the continuous phase, the organic solvent formed droplets similar to water-in-oil droplets in the device. In contrast to conventional microfluidic devices composed of resins, which are susceptible to swelling in organic solvents, the developed microfluidic device did not undergo swelling owing to the high chemical resistance of the constituent materials. Therefore, the device has potential applications for various chemical reactions involving organic solvents. Furthermore, this droplet generation device enabled control of droplet size by adjusting the liquid flow rate. The droplet generation method proposed in this work will contribute to the study of organic reactions in microdroplets and will be useful for evaluating scaling effects in various chemical reactions.

Quinoxaline derivatives demonstrate many distinguished chemical, biological, and physical properties and have a wide application in dyes, electroluminescent material, organic semiconductors, biological agents, etc. However, the synthesis of quinoxaline still suffers from several drawbacks, for instance, longer reaction time, unsatisfactory yields, and use of metal catalysts. Here, utilizing microdroplet-assisted reaction, we demonstrate the successive synthesis of several important quinoxaline derivatives. For case studies of 1H-indeno [1, 2-b] quinoxaline and 3,5-dimethyl-2-phenylquinoxaline, the present microdroplet approach can complete in milliseconds and the conversion rate reached 90% without adding any catalyst, which is considerably quicker and higher than conversional bulk-phase reactions. When combined with MS detection, high-throughput screening of the optimal reaction conditions can be achieved. Several impacts of droplet volume, reaction flow rate, distance from the MS inlet, spray voltage, and flow rate of the auxiliary gas can be screened on-site quickly for enhanced reaction speed and yields. More importantly, this platform is capable to be used for the scaled-up microdroplet synthesis of quinoxaline diversities. Considering the facile, economic, and environmentally friendly features of the microdroplet approach, we sincerely hope that the current strategy can effectively promote the academic research and industrial fabrications of functional quinoxaline substances for chemical, biological, and pharmaceutical application developments., (Copyright © 2020 Yang, Liu, Chen, Niu, Li, Niu, Yang, Mu and Tang.)

Disinfectants are important for arresting the spread of pathogens in the environment. Frequently used disinfectants are often incompatible with certain surfaces, expensive and can produce hazardous by-products. We report that micron-sized water droplets can act as an effective disinfectant, which were formed by spraying pure bulk water with coaxial nebulizing airflow. Spraying for 20 min onto Escherichia coli and Salmonella typhimurium on stainless-steel discs caused inactivation of over 98% of the bacteria. Control experiments resulted in less than 10% inactivation (water stream only and gas only) and 55% inactivation with 3% hydrogen peroxide. Experiments have shown that cell death results from cell wall destruction. We suggest that the combined action of reactive oxygen species present in water droplets (but not in bulk water) along with the droplet surface charge is responsible for the observed bactericidal activity., Competing Interests: The authors declare no conflict of interest., (© The Author(s) 2020. Published by Cambridge University Press 2020.)